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Ru catalyst nanoparticles were encapsulated into the pores of a Cr-based metal-organic framework (MOF)—MIL-101. The obtained material, as well as the non-loaded MIL-101, were investigated down to the atomic scale by annular dark-field scanning transmission electron microscopy using low dose conditions and fast image acquisition. The results directly show that the used wet chemistry loading approach is well-fitted for the accurate embedding of the individual catalyst nanoparticles into the cages of the MIL-101. The MIL-101 host material remains crystalline after the loading procedure, and the encapsulated Ru nanoparticles have a metallic nature. Annular dark field scanning transmission electron microscopy, combined with EDX mapping, is a perfect tool to directly characterize both the embedded nanoparticles and the loaded nanoscale MOFs. The resulting nanostructure of the material is promising because the Ru nanoparticles hosted in the MIL-101 pores are prevented from agglomeration—the stability and lifetime of the catalyst could be improved.
Maria Meledina; Geert Watson; Alexander Meledin; Pascal Van Der Voort; Joachim Mayer; Karen Leus. Ru Catalyst Encapsulated into the Pores of MIL-101 MOF: Direct Visualization by TEM. Materials 2021, 14, 4531 .
AMA StyleMaria Meledina, Geert Watson, Alexander Meledin, Pascal Van Der Voort, Joachim Mayer, Karen Leus. Ru Catalyst Encapsulated into the Pores of MIL-101 MOF: Direct Visualization by TEM. Materials. 2021; 14 (16):4531.
Chicago/Turabian StyleMaria Meledina; Geert Watson; Alexander Meledin; Pascal Van Der Voort; Joachim Mayer; Karen Leus. 2021. "Ru Catalyst Encapsulated into the Pores of MIL-101 MOF: Direct Visualization by TEM." Materials 14, no. 16: 4531.
C2/C1 hydrocarbon separation is an important industrial process that relies on energy-intensive cryogenic distillation methods. The use of porous adsorbents to selectively separate these gases is a viable alternative. Highly stable covalent triazine frameworks (urea-CTFs) have been synthesized using 1,3-bis(4-cyanophenyl)urea. Urea-CTFs exhibited gas uptakes of C2H2 (3.86 mmol/g) and C2H4 (2.92 mmol/g) at 273 K and 1 bar and is selective over CH4. Breakthrough simulations show the potential of urea-CTFs for C2/C1 separation.
Chidharth Krishnaraj; Himanshu Jena; Florence Lecoeuvre; Karen Leus; Pascal Van Der Voort. Rigid Nanoporous Urea-Based Covalent Triazine Frameworks for C2/C1 and CO2/CH4 Gas Separation. Molecules 2021, 26, 3670 .
AMA StyleChidharth Krishnaraj, Himanshu Jena, Florence Lecoeuvre, Karen Leus, Pascal Van Der Voort. Rigid Nanoporous Urea-Based Covalent Triazine Frameworks for C2/C1 and CO2/CH4 Gas Separation. Molecules. 2021; 26 (12):3670.
Chicago/Turabian StyleChidharth Krishnaraj; Himanshu Jena; Florence Lecoeuvre; Karen Leus; Pascal Van Der Voort. 2021. "Rigid Nanoporous Urea-Based Covalent Triazine Frameworks for C2/C1 and CO2/CH4 Gas Separation." Molecules 26, no. 12: 3670.
EPR spectra of V-doped DUT-5(Al) reveal four types of paramagnetic dopant species. Spin-Hamiltonian analysis and spectrum decomposition as function of V-content are supplemented with structural information from other spectroscopic techniques.
Kwinten Maes; Lisa I. D. J. Martin; Samira Khelifi; Alexander Hoffman; Karen Leus; Pascal Van Der Voort; Etienne Goovaerts; Philippe F. Smet; Veronique Van Speybroeck; Freddy Callens; Henk Vrielinck. Identification of vanadium dopant sites in the metal–organic framework DUT-5(Al). Physical Chemistry Chemical Physics 2021, 23, 7088 -7100.
AMA StyleKwinten Maes, Lisa I. D. J. Martin, Samira Khelifi, Alexander Hoffman, Karen Leus, Pascal Van Der Voort, Etienne Goovaerts, Philippe F. Smet, Veronique Van Speybroeck, Freddy Callens, Henk Vrielinck. Identification of vanadium dopant sites in the metal–organic framework DUT-5(Al). Physical Chemistry Chemical Physics. 2021; 23 (12):7088-7100.
Chicago/Turabian StyleKwinten Maes; Lisa I. D. J. Martin; Samira Khelifi; Alexander Hoffman; Karen Leus; Pascal Van Der Voort; Etienne Goovaerts; Philippe F. Smet; Veronique Van Speybroeck; Freddy Callens; Henk Vrielinck. 2021. "Identification of vanadium dopant sites in the metal–organic framework DUT-5(Al)." Physical Chemistry Chemical Physics 23, no. 12: 7088-7100.
Herein, a highly N-rich covalent triazine framework (CTF) is applied as support for a RuIII complex. The bipyridine sites within the CTF provide excellent anchoring points for the [Ru(acac)2(CH3CN)2]PF6 complex. The obtained robust [email protected] material was applied for the selective tandem aerobic oxidation–Knoevenagel condensation reaction. The presented system shows a high catalytic performance (>80% conversion of alcohols to α, β-unsaturated nitriles) without the use of expensive noble metals. The bipy-CTF not only acts as the catalyst support but also provides the active sites for both aerobic oxidation and Knoevenagel condensation reactions. This work highlights a new perspective for the development of highly efficient and robust heterogeneous catalysts applying CTFs for cascade catalysis.
Geert Watson; Parviz Gohari Derakhshandeh; Sara Abednatanzi; Johannes Schmidt; Karen Leus; Pascal Van Der Voort. A Ru-Complex Tethered to A N-Rich Covalent Triazine Framework for Tandem Aerobic Oxidation–Knoevenagel Condensation Reactions. Molecules 2021, 26, 838 .
AMA StyleGeert Watson, Parviz Gohari Derakhshandeh, Sara Abednatanzi, Johannes Schmidt, Karen Leus, Pascal Van Der Voort. A Ru-Complex Tethered to A N-Rich Covalent Triazine Framework for Tandem Aerobic Oxidation–Knoevenagel Condensation Reactions. Molecules. 2021; 26 (4):838.
Chicago/Turabian StyleGeert Watson; Parviz Gohari Derakhshandeh; Sara Abednatanzi; Johannes Schmidt; Karen Leus; Pascal Van Der Voort. 2021. "A Ru-Complex Tethered to A N-Rich Covalent Triazine Framework for Tandem Aerobic Oxidation–Knoevenagel Condensation Reactions." Molecules 26, no. 4: 838.
A novel strategy for toluene abatement was investigated using a sequential adsorption-regeneration process. Commercial Hopcalite (CuMn2Ox, Purelyst101MD), Ceria nanorods, and UiO-66-SO3H, a metal–organic framework (MOF), were selected for this study. Toluene was first adsorbed on the material and a mild thermal activation was performed afterwards in order to oxidize toluene into CO2 and H2O. The materials were characterized by XRD, N2 adsorption-desorption analysis, H2-TPR and TGA/DSC. The best dynamic toluene adsorption capacity was observed for UiO-66-SO3H due to its hierarchical porosity and high specific surface area. However, in terms of balance between storage and catalytic properties, Hopcalite stands out from others owing to its superior textural/chemical properties promoting irreversible toluene adsorption and outstanding redox properties, allowing a high activity and CO2 selectivity in toluene oxidation. The high conversion of toluene into CO2 which easily desorbs from the surface during heating treatment shows that the sequential adsorption-catalytic thermal oxidation can encompass a classical oxidation process in terms of efficiency, CO2 yield, and energy-cost saving, providing that the bifunctional material displays a good stability in repetitive working conditions.
Shilpa Sonar; Jean-Marc Giraudon; Savita Kaliya Perumal Veerapandian; Rim Bitar; Karen Leus; Pascal Van Der Voort; Jean-François Lamonier; Rino Morent; Nathalie De Geyter; Axel Löfberg. Abatement of Toluene Using a Sequential Adsorption-Catalytic Oxidation Process: Comparative Study of Potential Adsorbent/Catalytic Materials. Catalysts 2020, 10, 761 .
AMA StyleShilpa Sonar, Jean-Marc Giraudon, Savita Kaliya Perumal Veerapandian, Rim Bitar, Karen Leus, Pascal Van Der Voort, Jean-François Lamonier, Rino Morent, Nathalie De Geyter, Axel Löfberg. Abatement of Toluene Using a Sequential Adsorption-Catalytic Oxidation Process: Comparative Study of Potential Adsorbent/Catalytic Materials. Catalysts. 2020; 10 (7):761.
Chicago/Turabian StyleShilpa Sonar; Jean-Marc Giraudon; Savita Kaliya Perumal Veerapandian; Rim Bitar; Karen Leus; Pascal Van Der Voort; Jean-François Lamonier; Rino Morent; Nathalie De Geyter; Axel Löfberg. 2020. "Abatement of Toluene Using a Sequential Adsorption-Catalytic Oxidation Process: Comparative Study of Potential Adsorbent/Catalytic Materials." Catalysts 10, no. 7: 761.
The hybrid materials that are created by supporting or incorporating polyoxometalates (POMs) into/onto metal–organic frameworks (MOFs) have a unique set of properties. They combine the strong acidity, oxygen-rich surface, and redox capability of POMs, while overcoming their drawbacks, such as difficult handling, a low surface area, and a high solubility. MOFs are ideal hosts because of their high surface area, long-range ordered structure, and high tunability in terms of the pore size and channels. In some cases, MOFs add an extra dimension to the functionality of hybrids. This review summarizes the recent developments in the field of [email protected] hybrids. The most common applied synthesis strategies are discussed, together with major applications, such as their use in catalysis (organocatalysis, electrocatalysis, and photocatalysis). The more than 100 papers on this topic have been systematically summarized in a handy table, which covers almost all of the work conducted in this field up to now.
Jiamin Sun; Sara Abednatanzi; Pascal Van Der Voort; Ying-Ya Liu; Karen Leus. [email protected] Hybrids: Synthesis and Applications. Catalysts 2020, 10, 578 .
AMA StyleJiamin Sun, Sara Abednatanzi, Pascal Van Der Voort, Ying-Ya Liu, Karen Leus. [email protected] Hybrids: Synthesis and Applications. Catalysts. 2020; 10 (5):578.
Chicago/Turabian StyleJiamin Sun; Sara Abednatanzi; Pascal Van Der Voort; Ying-Ya Liu; Karen Leus. 2020. "[email protected] Hybrids: Synthesis and Applications." Catalysts 10, no. 5: 578.
Nitrogen-rich covalent triazine frameworks (CTFs) were grown in situ onto surface-functionalized carbon nanotubes. These novel hybrid catalysts electrochemically reduce CO2 to CO with a faradaic efficiency up to 81% at an overpotential of 380 mV.
Andreas Laemont; Sara Abednatanzi; Parviz Gohari Derakhshandeh; Florian Verbruggen; Erika Fiset; Qing Qin; Kevin Van Daele; Maria Meledina; Johannes Schmidt; Martin Oschatz; Pascal Van Der Voort; Korneel Rabaey; Markus Antonietti; Tom Breugelmans; Karen Leus. Covalent triazine framework/carbon nanotube hybrids enabling selective reduction of CO2 to CO at low overpotential. Green Chemistry 2020, 22, 3095 -3103.
AMA StyleAndreas Laemont, Sara Abednatanzi, Parviz Gohari Derakhshandeh, Florian Verbruggen, Erika Fiset, Qing Qin, Kevin Van Daele, Maria Meledina, Johannes Schmidt, Martin Oschatz, Pascal Van Der Voort, Korneel Rabaey, Markus Antonietti, Tom Breugelmans, Karen Leus. Covalent triazine framework/carbon nanotube hybrids enabling selective reduction of CO2 to CO at low overpotential. Green Chemistry. 2020; 22 (10):3095-3103.
Chicago/Turabian StyleAndreas Laemont; Sara Abednatanzi; Parviz Gohari Derakhshandeh; Florian Verbruggen; Erika Fiset; Qing Qin; Kevin Van Daele; Maria Meledina; Johannes Schmidt; Martin Oschatz; Pascal Van Der Voort; Korneel Rabaey; Markus Antonietti; Tom Breugelmans; Karen Leus. 2020. "Covalent triazine framework/carbon nanotube hybrids enabling selective reduction of CO2 to CO at low overpotential." Green Chemistry 22, no. 10: 3095-3103.
Rise of porous covalent triazine frameworks (CTFs) for sustainable applications.
Chidharth Krishnaraj; Himanshu Sekhar Jena; Karen Leus; Pascal Van Der Voort. Covalent triazine frameworks – a sustainable perspective. Green Chemistry 2020, 22, 1038 -1071.
AMA StyleChidharth Krishnaraj, Himanshu Sekhar Jena, Karen Leus, Pascal Van Der Voort. Covalent triazine frameworks – a sustainable perspective. Green Chemistry. 2020; 22 (4):1038-1071.
Chicago/Turabian StyleChidharth Krishnaraj; Himanshu Sekhar Jena; Karen Leus; Pascal Van Der Voort. 2020. "Covalent triazine frameworks – a sustainable perspective." Green Chemistry 22, no. 4: 1038-1071.
Synthesis, characterization and study of selective CO2 adsorption over other small gas molecules on a Zn-based porous framework compound.
Debraj Saha; Saikat Gayen; Tanmoy Maity; Antonio Frontera; Joaquín Ortega-Castro; Karen Leus; Guangbo Wang; Pascal Van Der Voort; Paula Brandão; Subratanath Koner. Combined experimental and computational studies on preferential CO2 adsorption over a zinc-based porous framework solid. New Journal of Chemistry 2019, 44, 1806 -1816.
AMA StyleDebraj Saha, Saikat Gayen, Tanmoy Maity, Antonio Frontera, Joaquín Ortega-Castro, Karen Leus, Guangbo Wang, Pascal Van Der Voort, Paula Brandão, Subratanath Koner. Combined experimental and computational studies on preferential CO2 adsorption over a zinc-based porous framework solid. New Journal of Chemistry. 2019; 44 (5):1806-1816.
Chicago/Turabian StyleDebraj Saha; Saikat Gayen; Tanmoy Maity; Antonio Frontera; Joaquín Ortega-Castro; Karen Leus; Guangbo Wang; Pascal Van Der Voort; Paula Brandão; Subratanath Koner. 2019. "Combined experimental and computational studies on preferential CO2 adsorption over a zinc-based porous framework solid." New Journal of Chemistry 44, no. 5: 1806-1816.
Invited for the cover of this issue is the group of Pascal Van Der Voort at the University of Ghent and colleagues at Technische Universität Berlin. The image depicts the covalent triazine frameworks reported in the manuscript for the sorption of CO2 and also in metal‐free catalysis. Read the full text of the article at 10.1002/chem.201903926.
Himanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Dr. Kristof Van Hecke; Dr. Pascal Van Der Voort. Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis. Chemistry – A European Journal 2019, 26, 1441 -1441.
AMA StyleHimanshu Sekhar Jena, Chidharth Krishnaraj, Johannes Schmidt, Karen Leus, Dr. Kristof Van Hecke, Dr. Pascal Van Der Voort. Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis. Chemistry – A European Journal. 2019; 26 (7):1441-1441.
Chicago/Turabian StyleHimanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Dr. Kristof Van Hecke; Dr. Pascal Van Der Voort. 2019. "Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis." Chemistry – A European Journal 26, no. 7: 1441-1441.
Himanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Dr. Kristof Van Hecke; Dr. Pascal Van Der Voort. Front Cover: Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis (Chem. Eur. J. 7/2020). Chemistry – A European Journal 2019, 26, 1437 -1437.
AMA StyleHimanshu Sekhar Jena, Chidharth Krishnaraj, Johannes Schmidt, Karen Leus, Dr. Kristof Van Hecke, Dr. Pascal Van Der Voort. Front Cover: Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis (Chem. Eur. J. 7/2020). Chemistry – A European Journal. 2019; 26 (7):1437-1437.
Chicago/Turabian StyleHimanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Dr. Kristof Van Hecke; Dr. Pascal Van Der Voort. 2019. "Front Cover: Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis (Chem. Eur. J. 7/2020)." Chemistry – A European Journal 26, no. 7: 1437-1437.
Herein, we report the construction of a set of fluorinated microporous covalent triazine frameworks (FCTFs) with appropriate CO2-philic functionalities (N and F) and high porosities for effective gas adsorption and separation.
Guangbo Wang; Yuliia Onyshchenko; Nathalie De Geyter; Rino Morent; Karen Leus; Pascal Van Der Voort. Straightforward preparation of fluorinated covalent triazine frameworks with significantly enhanced carbon dioxide and hydrogen adsorption capacities. Dalton Transactions 2019, 48, 17612 -17619.
AMA StyleGuangbo Wang, Yuliia Onyshchenko, Nathalie De Geyter, Rino Morent, Karen Leus, Pascal Van Der Voort. Straightforward preparation of fluorinated covalent triazine frameworks with significantly enhanced carbon dioxide and hydrogen adsorption capacities. Dalton Transactions. 2019; 48 (47):17612-17619.
Chicago/Turabian StyleGuangbo Wang; Yuliia Onyshchenko; Nathalie De Geyter; Rino Morent; Karen Leus; Pascal Van Der Voort. 2019. "Straightforward preparation of fluorinated covalent triazine frameworks with significantly enhanced carbon dioxide and hydrogen adsorption capacities." Dalton Transactions 48, no. 47: 17612-17619.
Covalent Triazine Frameworks (CTFs) have provided a unique platform in functional material design for a wide range of applications. Herein, we report a series of new CTFs with two new heteroaromatic building blocks (pyrazole and isoxazole groups) aiming for carbon capture and storage (CCS) and catalysis. The CTFs were synthesized from their respective building blocks [(4,4’‐(1H‐pyrazole‐3,5‐diyl)dibenzonitrile (pyz) and 4,4’‐(isoxazole‐3,5‐diyl)dibenzonitrile (isox))] under ionothermal conditions using ZnCl 2 . Both of the building blocks were designed by an organic transformation of an acetylacetone containing dinitrile linkers to pyrazole and isoxazole groups respectively. Due to this organic transformation, (i) linker aromatization, (ii) higher surface areas and nitrogen contents, (iii) higher aromaticity and (iv) higher surface basicity was achieved. Due to these enhanced properties, CTFs were explored for CO 2 uptake and metal free heterogeneous catalysis. Among all, the isox‐CTF, synthesized at 400 °C, showed the highest CO 2 uptake (4.92 mmol/g at 273K and 2.98 mmol/g at 298 K at 1 bar). Remarkably, these CTFs showed excellent metal‐free catalytic activity for the aerobic oxidation amine at mild reaction conditions. On studying the properties of the CTFs, it was observed that organic transformations and ligand aromatization of the materials are crucial factor to tune the important parameters that influence the CO 2 uptake and the catalytic activity.
Himanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Kristof Van Hecke; Pascal Van Der Voort. Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis. Chemistry – A European Journal 2019, 26, 1548 -1557.
AMA StyleHimanshu Sekhar Jena, Chidharth Krishnaraj, Johannes Schmidt, Karen Leus, Kristof Van Hecke, Pascal Van Der Voort. Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis. Chemistry – A European Journal. 2019; 26 (7):1548-1557.
Chicago/Turabian StyleHimanshu Sekhar Jena; Chidharth Krishnaraj; Johannes Schmidt; Karen Leus; Kristof Van Hecke; Pascal Van Der Voort. 2019. "Effect of Building Block Transformation in Covalent Triazine‐Based Frameworks for Enhanced CO 2 Uptake and Metal‐Free Heterogeneous Catalysis." Chemistry – A European Journal 26, no. 7: 1548-1557.
Covalent triazine frameworks (CTFs) are established as an emerging class of porous organic polymers with remarkable features such as large surface area and permanent porosity, high thermal and chemical stability, and convenient functionalization that promotes great potential in heterogeneous catalysis. In this article, we systematically present the structural design of CTFs as a versatile scaffold to develop heterogeneous catalysts for a variety of chemical reactions. We mainly focus on the functionalization of CTFs, including their use for incorporating and stabilization of nanoparticles and immobilization of molecular complexes onto the frameworks.
Norini Tahir; Chidharth Krishnaraj; Karen Leus; Pascal Van Der Voort. Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports. Polymers 2019, 11, 1326 .
AMA StyleNorini Tahir, Chidharth Krishnaraj, Karen Leus, Pascal Van Der Voort. Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports. Polymers. 2019; 11 (8):1326.
Chicago/Turabian StyleNorini Tahir; Chidharth Krishnaraj; Karen Leus; Pascal Van Der Voort. 2019. "Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports." Polymers 11, no. 8: 1326.
Aliphatic hexene-covalent triazine framework for C2/C1 hydrocarbon separation – dependence on morphology.
Chidharth Krishnaraj; Himanshu Sekhar Jena; Karen Leus; Helen M. Freeman; Liane G. Benning; Pascal Van Der Voort. An aliphatic hexene-covalent triazine framework for selective acetylene/methane and ethylene/methane separation. Journal of Materials Chemistry A 2019, 7, 13188 -13196.
AMA StyleChidharth Krishnaraj, Himanshu Sekhar Jena, Karen Leus, Helen M. Freeman, Liane G. Benning, Pascal Van Der Voort. An aliphatic hexene-covalent triazine framework for selective acetylene/methane and ethylene/methane separation. Journal of Materials Chemistry A. 2019; 7 (21):13188-13196.
Chicago/Turabian StyleChidharth Krishnaraj; Himanshu Sekhar Jena; Karen Leus; Helen M. Freeman; Liane G. Benning; Pascal Van Der Voort. 2019. "An aliphatic hexene-covalent triazine framework for selective acetylene/methane and ethylene/methane separation." Journal of Materials Chemistry A 7, no. 21: 13188-13196.
Mixed-metal MOFs contain at least 2 different metal ions presenting promising potential in heterogeneous catalysis, gas sorption/separation, luminescence and sensing.
Sara Abednatanzi; Parviz Gohari Derakhshandeh; Hannes Depauw; François-Xavier Coudert; Henk Vrielinck; Pascal Van Der Voort; Karen Leus. Mixed-metal metal–organic frameworks. Chemical Society Reviews 2019, 48, 2535 -2565.
AMA StyleSara Abednatanzi, Parviz Gohari Derakhshandeh, Hannes Depauw, François-Xavier Coudert, Henk Vrielinck, Pascal Van Der Voort, Karen Leus. Mixed-metal metal–organic frameworks. Chemical Society Reviews. 2019; 48 (9):2535-2565.
Chicago/Turabian StyleSara Abednatanzi; Parviz Gohari Derakhshandeh; Hannes Depauw; François-Xavier Coudert; Henk Vrielinck; Pascal Van Der Voort; Karen Leus. 2019. "Mixed-metal metal–organic frameworks." Chemical Society Reviews 48, no. 9: 2535-2565.
Xiao Feng; Himanshu Sekhar Jena; Karen Leus; Guangbo Wang; Judith Ouwehand; Pascal Van Der Voort. l-proline modulated zirconium metal organic frameworks: Simple chiral catalysts for the aldol addition reaction. Journal of Catalysis 2018, 365, 36 -42.
AMA StyleXiao Feng, Himanshu Sekhar Jena, Karen Leus, Guangbo Wang, Judith Ouwehand, Pascal Van Der Voort. l-proline modulated zirconium metal organic frameworks: Simple chiral catalysts for the aldol addition reaction. Journal of Catalysis. 2018; 365 ():36-42.
Chicago/Turabian StyleXiao Feng; Himanshu Sekhar Jena; Karen Leus; Guangbo Wang; Judith Ouwehand; Pascal Van Der Voort. 2018. "l-proline modulated zirconium metal organic frameworks: Simple chiral catalysts for the aldol addition reaction." Journal of Catalysis 365, no. : 36-42.
We present, for the first time, Covalent Triazine Frameworks functionalized with acetyl acetonate group (acac-CTFs). They are obtained from the polymerization of 4,4'-malonyldibenzonitrile under ionothermal conditions and exhibit BET surface areas up to 1626 m2/g. The materials show excellent CO2 uptake (3.30 mmol/g at 273 K and 1 bar), H2 storage capacity (1.53 wt% at 77 K and 1 bar) and a good CO2/N2 selectivity (up to 46 at 298 K). The enhanced CO2 uptake value and good selectivity are due to the presence of dual polar sites (N and O) throughout the material. In addition, acac-CTF was used to anchor VO(acac)2 as a heterogeneous catalyst. The [email protected] showed outstanding reactivity and reusability for the modified Mannich-type reaction with a higher turnover number than the homogeneous catalyst. The higher reactivity and reusability of the catalyst comes from the coordination of the vanadyl ions to the acetyl acetonate groups present in the material. The strong metalation is confirmed from Fourier Transform Infrared analysis, 13C MAS NMR spectral analysis and X-ray photoelectron spectroscopy measurement. Detailed characterization of the [email protected] reveals that electron donation from O^O of the acetyl acetonate group to VO(acac)2, combined with the very high surface area of acac-CTF, is responsible for the stabilization of the catalyst. Overall, this contribution highlights the necessity of stable catalytic binding sites on heterogeneous supports to fabricate greener catalysts for sustainable chemistry.
Himanshu Sekhar Jena; Chidharth Krishnaraj; Guangbo Wang; Karen Leus; Johannes Schmidt; Nicolas Chaoui; Pascal Van Der Voort. Acetylacetone Covalent Triazine Framework: An Efficient Carbon Capture and Storage Material and a Highly Stable Heterogeneous Catalyst. Chemistry of Materials 2018, 30, 4102 -4111.
AMA StyleHimanshu Sekhar Jena, Chidharth Krishnaraj, Guangbo Wang, Karen Leus, Johannes Schmidt, Nicolas Chaoui, Pascal Van Der Voort. Acetylacetone Covalent Triazine Framework: An Efficient Carbon Capture and Storage Material and a Highly Stable Heterogeneous Catalyst. Chemistry of Materials. 2018; 30 (12):4102-4111.
Chicago/Turabian StyleHimanshu Sekhar Jena; Chidharth Krishnaraj; Guangbo Wang; Karen Leus; Johannes Schmidt; Nicolas Chaoui; Pascal Van Der Voort. 2018. "Acetylacetone Covalent Triazine Framework: An Efficient Carbon Capture and Storage Material and a Highly Stable Heterogeneous Catalyst." Chemistry of Materials 30, no. 12: 4102-4111.
The covalent triazine framework, CTF-1, served as host material for the in situ synthesis of Fe2O3 nanoparticles. The composite material consisted of 20 ± 2 m% iron, mainly in γ-Fe2O3 phase. The resulting γ[email protected] was examined for the adsorption of AsIII, AsV and HgII from synthetic solutions and real surface-, ground- and wastewater. The material shows excellent removal efficiencies, independent from the presence of Ca2+, Mg2+ or natural organic matter and only limited dependency on the presence of phosphate ions. Its adsorption capacity towards arsenite (198.0 mg g−1), arsenate (102.3 mg g−1) and divalent mercury (165.8 mg g−1) belongs amongst the best-known adsorbents, including many other iron-based materials. Regeneration of the adsorbent can be achieved for use over multiple cycles without a decrease in performance by elution at 70 °C with 0.1 M NaOH, followed by a stirring step in a 5 m% H2O2 solution for As or 0.1 M thiourea and 0.001 M HCl for Hg. In highly contaminated water (100 μg L−1), the adsorbent polishes the water quality to well below the current WHO limits.
Karen Leus; Karel Folens; Nina Ricci Nicomel; Jeffrey Paulo Perez; Maria Filippousi; Maria Meledina; Marinela M. Dîrtu; Stuart Turner; Gustaaf Van Tendeloo; Yann Garcia; Gijs Du Laing; Pascal Van Der Voort. Removal of arsenic and mercury species from water by covalent triazine framework encapsulated γ-Fe2O3 nanoparticles. Journal of Hazardous Materials 2018, 353, 312 -319.
AMA StyleKaren Leus, Karel Folens, Nina Ricci Nicomel, Jeffrey Paulo Perez, Maria Filippousi, Maria Meledina, Marinela M. Dîrtu, Stuart Turner, Gustaaf Van Tendeloo, Yann Garcia, Gijs Du Laing, Pascal Van Der Voort. Removal of arsenic and mercury species from water by covalent triazine framework encapsulated γ-Fe2O3 nanoparticles. Journal of Hazardous Materials. 2018; 353 ():312-319.
Chicago/Turabian StyleKaren Leus; Karel Folens; Nina Ricci Nicomel; Jeffrey Paulo Perez; Maria Filippousi; Maria Meledina; Marinela M. Dîrtu; Stuart Turner; Gustaaf Van Tendeloo; Yann Garcia; Gijs Du Laing; Pascal Van Der Voort. 2018. "Removal of arsenic and mercury species from water by covalent triazine framework encapsulated γ-Fe2O3 nanoparticles." Journal of Hazardous Materials 353, no. : 312-319.
Metal Organic Frameworks (MOFs) have been explored widely to create heterogeneity in a catalytic system. Catalytic applications require the use of stable catalysts with no leaching and easy recovery. In this regard, [email protected] is embedded in a poly-є-caprolactone (PCL) matrix by means of electrospinning to create a “catalytic carpet” which is highly efficient and can be recovered within seconds after catalysis. The obtained composite material is completely intact with a homogeneous distribution of the [email protected] throughout the electrospun PCL fiber matrix. The catalytic carpet was examined in the hydrogenation of cyclohexene and full conversion was obtained in just 90 min. Remarkably, a very large fraction (>65%) of the total Pt-atoms participate in the reaction. Reusability tests showed that the material could be recycled for at least 4 runs without detectable Cr and Pt leaching displaying the durability of the catalytic carpets. Complete recovery is achieved with zero weight loss while fully preserving the crystalline structure.
Karen Leus; Chidharth Krishnaraj; Luca Verhoeven; Véronique Cremers; Jolien Dendooven; Ranjith K. Ramachandran; Peter Dubruel; Pascal Van Der Voort. Catalytic carpets: [email protected]@electrospun PCL, a surprisingly active and robust hydrogenation catalyst. Journal of Catalysis 2018, 360, 81 -88.
AMA StyleKaren Leus, Chidharth Krishnaraj, Luca Verhoeven, Véronique Cremers, Jolien Dendooven, Ranjith K. Ramachandran, Peter Dubruel, Pascal Van Der Voort. Catalytic carpets: [email protected]@electrospun PCL, a surprisingly active and robust hydrogenation catalyst. Journal of Catalysis. 2018; 360 ():81-88.
Chicago/Turabian StyleKaren Leus; Chidharth Krishnaraj; Luca Verhoeven; Véronique Cremers; Jolien Dendooven; Ranjith K. Ramachandran; Peter Dubruel; Pascal Van Der Voort. 2018. "Catalytic carpets: [email protected]@electrospun PCL, a surprisingly active and robust hydrogenation catalyst." Journal of Catalysis 360, no. : 81-88.