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2. Charge transport modulation by a redox supramolecular spin-filtering chiral crystal

Author

Verhage, Michael, Bampoulis, Pantelis, Preuss, Marco D., Filot, Ivo, Friedrich, Heiner, Joosten, Rick R. M., Meijer, E. W., and Flipse, Kees

Subjects
Condensed Matter - Materials Science, Condensed Matter - Mesoscale and Nanoscale Physics
Abstract

The chirality induced spin selectivity (CISS) effect is a fascinating phenomena correlating molecular structure with electron spin-polarisation in excited state measurements. Experimental procedures to quantify the spin-filtering magnitude relies generally on averaging data sets, especially those from magnetic field dependent conductive-AFM. We investigate the underlying observed disorder in the IV spectra and the origin of spikes superimposed. We demonstrate and explain that a dynamic, voltage sweep rate dependent, phenomena can give rise to complex IV curves for chiral crystals of coronene bisimide. The redox group, able to capture localized charge states, acts as an impurity state interfering with a continuum, giving rise to Fano resonances. We introduce a novel mechanism for the dynamic transport which might also provide insight into the role of spin-polarization. Crucially, interference between charge localisation and delocalisation during transport may be important properties into understanding the CISS phenomena.

Published
2023

3. What Happens at Surfaces and Grain Boundaries of Halide Perovskites: Insights from Reactive Molecular Dynamics Simulations of CsPbI$_{3}$

Author

Pols, Mike, Hilpert, Tobias, Filot, Ivo, van Duin, Adri C. T., Calero, Sofía, and Tao, Shuxia

Subjects
Condensed Matter - Materials Science
Abstract

The commercialization of perovskite solar cells is hindered by the poor long-term stability of the metal halide perovskite (MHP) light absorbing layer. Solution processing, the common fabrication method for MHPs, produces polycrystalline films with a wide variety of defects, such as point defects, surfaces, and grain boundaries. Although the optoelectronic effects of such defects have been widely studied, the evaluation of their impact on the long-term stability remains challenging. In particular, an understanding of the dynamics of degradation reactions at the atomistic scale is lacking. In this work, using reactive force field (ReaxFF) molecular dynamics simulations, we investigate the effects of defects, in the forms of surfaces, surface defects and grain boundaries, on the stability of the inorganic halide perovskite CsPbI$_{3}$. Our simulations establish a stability trend for a variety of surfaces, which correlates well with the occurrence of these surfaces in experiments. We find that a perovskite surface degrades by progressively changing the local geometry of PbI$_{\mathrm{x}}$ octahedra from corner- to edge- to face-sharing. Importantly, we find that Pb dangling bonds and the lack of steric hindrance of I species are two crucial factors that induce degradation reactions. Finally, we show that the stability of these surfaces can be modulated by adjusting their atomistic details, either by creating additional point defects or merging them to form grain boundaries. While in general additional defects, particularly when clustered, have a negative impact on the material stability, some grain boundaries have a stabilizing effect, primarily because of the additional steric hindrance., Comment: 29 pages, 7 figures

Published
2022
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6. Atomistic insights into the degradation of halide perovskites: a reactive force field molecular dynamics study

Author

Pols, Mike, Vicent-Luna, José Manuel, Filot, Ivo, van Duin, Adri C. T., and Tao, Shuxia

Subjects
Condensed Matter - Materials Science
Abstract

Halide perovskites make efficient solar cells due to their exceptional optoelectronic properties, but suffer from several stability issues. The characterization of the degradation processes is challenging because of the limitations in the spatio-temporal resolution in experiments and the absence of efficient computational methods to study the reactive processes. Here, we present the first effort in developing reactive force fields for large scale molecular dynamics simulations of the phase instability and the defect-induced degradation reactions in inorganic CsPbI$_{3}$. We find that the phase transitions are driven by a combination of the anharmonicity of the perovskite lattice with the thermal entropy. At relatively low temperatures, the Cs cations tend to move away from the preferential positions with good contacts with the surrounding metal halide framework, potentially causing its conversion to a non-perovskite phase. Our simulations of defective structures reveal that, although both iodine vacancies and interstitials are very mobile in the perovskite lattice, the vacancies have a detrimental effect on the stability, initiating the decomposition reactions of perovskites to PbI$_{2}$. Our work puts ReaxFF forward as an effective computational framework to study reactive processes in halide perovskites., Comment: 11 pages, 6 figures

Published
2021
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11. 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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14. Descriptor for C2N-Supported Single-Cluster Catalysts in Bifunctional Oxygen Evolution and Reduction Reactions

Author

Pan, Jing, Li, Min, Filot, Ivo A.W., Wang, Hui, Hensen, Emiel J.M., Zhang, Long, Pan, Jing, Li, Min, Filot, Ivo A.W., Wang, Hui, Hensen, Emiel J.M., and Zhang, Long

Abstract

Developing highly active cluster catalysts for the bifunctional oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is significant for future renewable energy technology. Here, we employ first-principles calculations combined with a genetic algorithm to explore the activity trends of transition metal clusters supported on C2N. Our results indicate that the supported clusters, as bifunctional catalysts for the OER and the ORR, may outperform single-atom catalysts. In particular, the C2N-supported Ag6 cluster exhibits outstanding bifunctional activity with low overpotentials. Mechanistic analysis indicates that the activity of the cluster is related to the number of atoms in the active site as well as the interaction between the intermediate and the cluster. Accordingly, we identify a descriptor that links the intrinsic properties of the clusters with the activity of both the OER and the ORR. This work provides guidelines and strategies for the rational design of highly efficient bifunctional cluster catalysts.

Published
2024

25. Understanding carbon dioxide activation and carbon–carbon coupling over nickel

Author

Charlotte Vogt, Matteo Monai, Ellen B. Sterk, Jonas Palle, Angela E. M. Melcherts, Bart Zijlstra, Esther Groeneveld, Peter H. Berben, Jelle M. Boereboom, Emiel J. M. Hensen, Florian Meirer, Ivo A. W. Filot, and Bert M. Weckhuysen

Subjects
Science
Abstract

Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide and higher hydrocarbons, but needs improved catalysts. Here, the authors use a combined theoretical and experimental approach to tune the activity and selectivity of CO2 conversion over nickel towards desired products.

Published
2019
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29. On the Potential of Gallium- and Indium-Based Liquid Metal Membranes for Hydrogen Separation

Author

Leon R. S. Rosseau, José A. Medrano, Rajat Bhardwaj, Earl L. V. Goetheer, Ivo A. W. Filot, Fausto Gallucci, and Martin van Sint Annaland

Subjects
dense metal membrane, microkinetics, Sieverts’ law, hydrogen, liquid metals, Chemical technology, TP1-1185, Chemical engineering, TP155-156
Abstract

The concept of liquid metal membranes for hydrogen separation, based on gallium or indium, was recently introduced as an alternative to conventional palladium-based membranes. The potential of this class of gas separation materials was mainly attributed to the promise of higher hydrogen diffusivity. The postulated improvements are only beneficial to the flux if diffusion through the membrane is the rate-determining step in the permeation sequence. Whilst this is a valid assumption for hydrogen transport through palladium-based membranes, the relatively low adsorption energy of hydrogen on both liquid metals suggests that other phenomena may be relevant. In the current study, a microkinetic modeling approach is used to enable simulations based on a five-step permeation mechanism. The calculation results show that for the liquid metal membranes, the flux is limited by the dissociative adsorption over a large temperature range, and that the membrane flux is expected to be orders of magnitude lower compared to the membrane flux through pure palladium membranes. Even when accounting for the lower cost of the liquid metals compared to palladium, the latter still outperforms both gallium and indium in all realistic scenarios, in part due to the practical difficulties associated with making liquid metal thin films.

Published
2022
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34. Computational study of CO2 methanation on Ru/CeO2 model surfaces: On the impact of Ru doping in CeO2

Author

Chen, Lulu, Filot, Ivo A.W., Hensen, Emiel J.M., Chen, Lulu, Filot, Ivo A.W., and Hensen, Emiel J.M.

Abstract

The Sabatier reaction (CO 2 + H 2 → CH 4 + H 2O) can contribute to renewable energy storage by converting green H 2 with waste CO 2 into CH 4. Highly dispersed Ru on CeO 2 represents an active catalyst for the CO 2 methanation. Here, we investigated the support effect by considering a single atom of Ru and a small Ru cluster on CeO 2 (Ru 6/CeO 2). The influence of doping CeO 2 with Ru was investigated as well (Ru 6/RuCe x-1O 2x-1). Density functional theory was used to compute the reaction energy diagrams. A single Ru atom on CeO 2 can only break one of the C-O bonds in adsorbed CO 2, making it only active in the reverse water-gas shift reaction. In contrast, Ru 6 clusters on stoichiometric and Ru-doped CeO 2 are active methanation catalysts. CO is the main reaction intermediate formed via a COOH surface intermediate. Compared to an extended Ru(11-21) surface containing step-edge sites where direct C-O bond dissociation is facile, C-O dissociation proceeds via H-assisted pathways (CO → HCO → CH) on Ru 6/CeO 2 and Ru 6/RuCe x-1O 2x-1. A higher CO 2 methanation rate is predicted for Ru 6/RuCe x-1O 2x-1. Electronic structure analysis clarifies that the lower activation energy for HCO dissociation on Ru 6/RuCe x-1O 2x-1 is caused by stronger electron-electron repulsion due to its closer proximity to Ru. Strong H 2 adsorption on small Ru clusters explains the higher CO 2 methanation activity of Ru clusters on CeO 2 compared to a Ru step-edge surface, representative of Ru nanoparticles, where the H coverage is low due to stronger competition with adsorbed CO.

Published
2023

35. Elucidation of the Reverse Water-Gas Shift Reaction Mechanism over an Isolated Ru Atom on CeO2(111)

Author

Chen, Lulu, Filot, Ivo A.W., Hensen, Emiel J.M., Chen, Lulu, Filot, Ivo A.W., and Hensen, Emiel J.M.

Abstract

Ru/CeO2 single-atom catalysts (SAC) are highly selective for the hydrogenation of CO2 to CO. In this study, we developed a molecular-level understanding of the reverse water–gas shift (rWGS) reaction over Ru/CeO2 SAC using density functional theory in conjunction with microkinetic modeling. A reaction mechanism network involving different Ru states was constructed. Starting from a Ru single atom coordinating to three lattice oxygen atoms of ceria (denoted as RuO3), RuO3 can be hydrogenated to Ru(OH)3-(OH) through hydrogen spillover or reduced to RuO2(Ov). Direct and H-assisted CO2 dissociation mechanisms are taken into account. Microkinetics simulations indicate that Ru(OH)3-(OH) is the dominant active site in the low-temperature regime. The presence of hydroxyl species in Ru(OH)3-(OH) promotes the dissociation of CO2 and water formation. The promoting effect of hydroxyl groups is caused by enhanced charge donation of Ru to antibonding orbitals of CO2. At elevated temperatures, a Mars-van Krevelen mechanism is preferred due to the facile formation of oxygen vacancies. Overall, our findings provide insight into the role of spillover H species in the rWGS reaction on Ru/CeO2 SAC and the change in active sites with reaction temperature.

Published
2023

36. Effect of reaction atmosphere on catalytic CO oxidation over Cu-based bimetallic nanoclusters on a CeO2 support

Author

Zhang, Long, Pan, Jing, Li, Min, Filot, Ivo A.W., Hensen, Emiel J.M., Wang, Hui, Zhang, Long, Pan, Jing, Li, Min, Filot, Ivo A.W., Hensen, Emiel J.M., and Wang, Hui

Abstract

Understanding the nature of active sites and the catalytic properties of oxide-supported bimetallic clusters under reaction conditions remains challenging. In this study, we combine first-principles calculations with genetic algorithm and grand canonical Monte Carlo methods to reveal the structures and compositions of CeO2-supported Cu-based bimetallic clusters in an oxygen-rich environment. Oxidized Cu4X4 (X = Pd, Pt, and Rh) bimetallic clusters on CeO2(111) are stable and exhibit different catalytic properties during CO oxidation compared with the pristine bimetallic clusters. Microkinetic simulations predict that CeO2(111)-supported Cu4Pd4O10, Cu4Pt4O11, and Cu4Rh4O14 clusters have much higher CO oxidation activity than the supported Cu4Pd4, Cu4Pt4, and Cu4Rh4 clusters; this is ascribed to the moderate CO adsorption strength and active oxygen on oxidized alloy clusters. A mechanistic study suggests that CO oxidation occurs via the O2 associative reaction mechanism on the Cu4Pd4O10 and Cu4Pt4O11 clusters, while it proceeds through the O2 dissociative reaction mechanism on the Cu4Rh4O14 cluster. Our calculations further predict that CO oxidation on the Cu4Rh4O14 cluster exhibits a low apparent activation energy, indicating that the oxidized cluster possesses excellent CO oxidation activity. This work demonstrates that the catalytic activity and reaction mechanism vary with the composition and oxidation state of the alloy nanocluster under the reaction conditions and emphasizes the influence of the reaction atmosphere on the reaction mechanisms and catalytic activity of oxide-supported alloy catalysts.

Published
2023

37. A computational study of CO2 hydrogenation on single atoms of Pt, Pd, Ni and Rh on In2O3(111)

Author

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

Abstract

Metal promoted indium oxide (In2O3) catalysts are promising materials for CO2 hydrogenation to products such as methanol and carbon monoxide. The influence of the dispersion of the promoting metal on the methanol selectivity of In2O3 catalysts 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 CO2 hydrogenation to CO and methanol. Direct and hydrogen-assisted CO2 dissociation pathways leading to CO as well as methanol formation via either formate or CO intermediates are explicitly considered. Microkinetic simulations show that all SA models mainly catalyze CO formation via a redox pathway involving oxygen vacancies where adsorbed CO2 dissociates 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

38. Unraveling the Role of Metal-Support Interactions on the Structure Sensitivity of Fischer-Tropsch Synthesis

Author

van Etten, Michel P.C., de Laat, Michelle E., Hensen, Emiel J.M., Filot, Ivo A.W., van Etten, Michel P.C., de Laat, Michelle E., Hensen, Emiel J.M., and Filot, Ivo A.W.

Abstract

Structure sensitivity plays a pivotal role in heterogeneous catalysis and the Fischer-Tropsch reaction is one of the prime examples of such a structure-sensitive reaction. The activity and selectivity of this reaction depend on the size of the nanoparticle and this trend is observed for a whole range of support materials. To understand why metal-support interactions do not affect this trend, a ReaxFF force field is developed that effectively mimics the broad variety of support materials and captures the metal-support interaction strength into a single structural parameter. Particles of 1-9 nm embedded on support materials are sampled using simulated annealing molecular dynamics and the effect of the metal-support interaction on the active site distribution is studied. It is found that although the size-dependency profile of various active site topologies depends on the interaction strength of the nanoparticle with the support, step-edge sites with an FCC(110) motif remain insensitive to the type of support. Based on microkinetic simulations, it is established that these sites are predominantly responsible for the observed atom-based FTS activity rationalizing why Fischer-Tropsch synthesis is structure-sensitive but support-insensitive.

Published
2023

39. The Promoting Role of Ni on In2O3 for CO2 Hydrogenation to Methanol

Author

Cannizzaro, Francesco, Hensen, Emiel J.M., Filot, Ivo A.W., Cannizzaro, Francesco, Hensen, Emiel J.M., and Filot, Ivo A.W.

Abstract

Ni-promoted indium oxide (In2O3) is a promising catalyst for the selective hydrogenation of CO2 to CH3OH, but the nature of the active Ni sites remains unknown. By employing density functional theory and microkinetic modeling, we elucidate the promoting role of Ni in In2O3-catalyzed CO2 hydrogenation. Three representative models have been investigated: (i) a single Ni atom doped in the In2O3(111) surface, (ii) a Ni atom adsorbed on In2O3(111), and (iii) a small cluster of eight Ni atoms adsorbed on In2O3(111). Genetic algorithms (GAs) are used to identify the optimum structure of the Ni8 clusters on the In2O3 surface. Compared to the pristine In2O3(111) surface, the Ni8-cluster model offers a lower overall barrier to oxygen vacancy formation, whereas, on both single-atom models, higher overall barriers are found. Microkinetic simulations reveal that only the supported Ni8 cluster can lead to high methanol selectivity, whereas single Ni atoms either doped in or adsorbed on the In2O3 surface mainly catalyze CO formation. Hydride species obtained by facile H2 dissociation on the Ni8 cluster are involved in the hydrogenation of adsorbed CO2 to formate intermediates and methanol. At higher temperatures, the decreasing hydride coverage shifts the selectivity to CO. On the Ni8-cluster model, the formation of methane is inhibited by high barriers associated with either direct or H-assisted CO activation. A comparison with a smaller Ni6 cluster also obtained with GAs exhibits similar barriers for key rate-limiting steps for the formation of CO, CH4, and CH3OH. Further microkinetic simulations show that this model also has appreciable selectivity to methanol a

Published
2023

41. Lateral Interactions of Dynamic Adlayer Structures from Artificial Neural Networks

Author

Bart Klumpers, Ivo Filot, Emiel Hensen, Inorganic Materials & Catalysis, EIRES Chem. for Sustainable Energy Systems, and EAISI Foundational

Subjects
General Energy, Physical and Theoretical Chemistry, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials
Abstract

Lateral interactions are a key factor in the correct description of adsorption isotherms relevant to heterogeneous catalytic reactions. To model these lateral interactions, a large number of monolayer structures have to be investigated, far exceeding the limitations of conventional techniques such as density functional theory. We have developed a new hybrid neural network model that can substitute the electronic structure calculations for these monolayer structures, without significant loss of accuracy. The low computational cost of this model allows the study of the adlayer structures close to industrial operating conditions. Lateral interactions are found to increase at elevated temperatures as a result of increased adsorbate mobility, and this contribution is found to be key in unifying theoretical and experimental observations. We show that the inclusion of dispersion interactions in stabilizing the adlayers is necessary to obtain correct predictions for both isotherms and adsorption site distributions.

Published
2022

42. 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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47. The Promoting Role of Ni on In2O3 for CO2 Hydrogenation to Methanol

Author

Ivo Filot, Emiel Hensen, Francesco Cannizzaro, Inorganic Materials & Catalysis, EIRES Chem. for Sustainable Energy Systems, and EAISI Foundational

Subjects
CO hydrogenation, Ni, InO, mechanism, General Chemistry, oxygen vacancy, Catalysis
Abstract

Ni-promoted indium oxide (In2O3) is a promising catalyst for the selective hydrogenation of CO2 to CH3OH, but the nature of the active Ni sites remains unknown. By employing density functional theory and microkinetic modeling, we elucidate the promoting role of Ni in In2O3-catalyzed CO2 hydrogenation. Three representative models have been investigated: (i) a single Ni atom doped in the In2O3(111) surface, (ii) a Ni atom adsorbed on In2O3(111), and (iii) a small cluster of eight Ni atoms adsorbed on In2O3(111). Genetic algorithms (GAs) are used to identify the optimum structure of the Ni8 clusters on the In2O3 surface. Compared to the pristine In2O3(111) surface, the Ni8-cluster model offers a lower overall barrier to oxygen vacancy formation, whereas, on both single-atom models, higher overall barriers are found. Microkinetic simulations reveal that only the supported Ni8 cluster can lead to high methanol selectivity, whereas single Ni atoms either doped in or adsorbed on the In2O3 surface mainly catalyze CO formation. Hydride species obtained by facile H2 dissociation on the Ni8 cluster are involved in the hydrogenation of adsorbed CO2 to formate intermediates and methanol. At higher temperatures, the decreasing hydride coverage shifts the selectivity to CO. On the Ni8-cluster model, the formation of methane is inhibited by high barriers associated with either direct or H-assisted CO activation. A comparison with a smaller Ni6 cluster also obtained with GAs exhibits similar barriers for key rate-limiting steps for the formation of CO, CH4, and CH3OH. Further microkinetic simulations show that this model also has appreciable selectivity to methanol at low temperatures. The formation of CO over single Ni atoms either doped in or adsorbed on the In2O3 surface takes place via a redox pathway involving the formation of oxygen vacancies and direct CO2 dissociation.

Published
2023

48. 6.16 - Promoted Fischer-Tropsch catalysts

Author

Webb, Paul, Filot, Ivo A.W., EAISI Foundational, and Inorganic Materials & Catalysis

Abstract

Fischer-Tropsch synthesis (FTS) is the conversion of synthesis gas, a mixture of carbon monoxide and hydrogen, into a broad range of hydrocarbon products, including olefins, paraffins and oxygenates. The process is essentially a polymerization reaction involving the stepwise coupling of C1 monomeric units that are generated in situ from CO and H2. Careful design of catalyst and process parameters allows for selectivity control and the production of a versatile range of fuels and chemicals. In this chapter, a brief historical overview will be given, from the early discoveries of Frans Fischer and Hans Tropsch up to present day state-of-the-art commercial processes. Features of catalyst structure, preparation and performance will be discussed in detail and followed by a contemporary overview of the kinetic mechanism and structure-sensitivity of the reaction. These mechanistic insights provide the basis for a “smart design” approach to next generation catalysts. Concepts for tuning selectively to high-value chemicals, such as olefins and higher alcohols, will be discussed and the chapter will conclude with a brief outlook on the future role of FTS in a post-fossil fuel world.

Published
2023

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