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Wang, R. (author), Sun, X. (author), Ould-Chikh, Samy (author), Osadchii, D. (author), Bai, F. (author), Kapteijn, F. (author), Gascon, Jorge (author)
A nitrogen-doped carbon was synthesized through the pyrolysis of the well-known metal-organic framework ZIF-8, followed by a subsequent acid treatment, and has been applied as a catalyst in the electrochemical reduction of carbon dioxide. The resulting electrode shows Faradaic efficiencies to carbon monoxide as high as ∼78%, with hydrogen...
journal article 2018
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Etxeberria Benavides, M. (author), David, Oana (author), Johnson, Timothy (author), Łozińska, Magdalena M. (author), Orsi, Angelica (author), Wright, Paul A. (author), Mastel, Stefan (author), Hillenbrand, Rainer (author), Kapteijn, F. (author), Gascon, Jorge (author)
Carbon capture and storage (CCS) using membranes for the separation of CO<sub>2</sub> holds great promise for the reduction of atmospheric CO<sub>2</sub> emissions from fuel combustion and industrial processes. Among the different process outlines, post-combustion CO<sub>2</sub> capture could be easily implemented in existing power plants....
journal article 2018
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Goetze, Joris (author), Yarulina, I. (author), Gascon, Jorge (author), Kapteijn, F. (author), Weckhuysen, Bert M. (author)
In small-pore zeolite catalysts, where the size of the pores is limited by eight-ring windows, aromatic hydrocarbon pool molecules that are formed inside the zeolite during the Methanol-to-Olefins (MTO) process cannot exit the pores and are retained inside the catalyst. Hydrocarbon species whose size is comparable to the size of the zeolite...
journal article 2018
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Vollmer, I. (author), van der Linden, B. (author), Ould-Chikh, Samy (author), Aguilar-Tapia, Antonio (author), Yarulina, I. (author), Abou-Hamad, Edy (author), Sneider, Yuri G. (author), Olivos Suarez, A.I. (author), Hazemann, Jean-Louis (author), Kapteijn, F. (author), Gascon, Jorge (author)
The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active...
journal article 2018
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Sabetghadam, Anahid (author), Liu, X. (author), Benzaqui, Marvin (author), Gkaniatsou, Effrosyni (author), Orsi, Angelica (author), Lozinska, Magdalena M. (author), Sicard, Clemence (author), Johnson, Timothy (author), Steunou, Nathalie (author), Wright, Paul A. (author), Serre, Christian (author), Gascon, Jorge (author), Kapteijn, F. (author)
To gain insight into the influence of metal-organic framework (MOF) fillers and polymers on membrane performance, eight different composites were studied by combining four MOFs and two polymers. MOF materials (NH<sub>2</sub>-MIL-53(Al), MIL-69(Al), MIL-96(Al) and ZIF-94) with various chemical functionalities, topologies, and dimensionalities...
journal article 2018
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Szécsényi, Ágnes (author), Li, G. (author), Gascon, Jorge (author), Pidko, E.A. (author)
Periodic density functional theory (DFT) calculations were carried out to investigate the mechanism of methane oxidation with H<sub>2</sub>O<sub>2</sub> over the defined Fe sites in Fe/ZSM-5 zeolite. The initial Fe site is modeled as a [(H<sub>2</sub>O)<sub>2</sub>-Fe(III)-(μO)<sub>2</sub>-Fe(III)-(H<sub>2</sub>O)<sub>2</sub>]<sup>2+</sup>...
journal article 2018
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Shan, M. (author), Seoane, Beatriz (author), Pustovarenko, Alexey (author), Wang, X. (author), Liu, X. (author), Yarulina, I. (author), Abou-Hamad, Edy (author), Kapteijn, F. (author), Gascon, Jorge (author)
The performance of mixed-matrix membranes (MMMs) based on Matrimid<sup>®</sup> and benzimidazole-linked polymers (BILPs) have been investigated for the separation CO<sub>2</sub>/N<sub>2</sub> and the dependency on the filler porosity. BILPs with two different porosities (BILP-101 and RT-BILP-101) were synthesized through controlling the...
journal article 2018
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Szécsényi, A. (author), Li, G. (author), Gascon, Jorge (author), Pidko, E.A. (author)
Reaction paths underlying the catalytic oxidation of methane with H<sub>2</sub>O<sub>2</sub> over an Fe containing MIL-53(Al) metal-organic framework were studied by periodic DFT calculations. Not only the activation of methane, but the full reaction network was considered, which includes the formation of the active site, the overoxidation of...
journal article 2018
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Vollmer, I. (author), Li, G. (author), Yarulina, I. (author), Kosinov, N. (author), Hensen, Emiel J. (author), Houben, Klaartje (author), Mance, Deni (author), Baldus, Marc (author), Gascon, Jorge (author), Kapteijn, F. (author)
Although the local geometry of Mo in Mo/HZSM-5 has been characterized before, we present a systematic way to manipulate the configuration of Mo and link it to its catalytic properties. The location and geometry of cationic Mo-complexes, the precursor of the active metal site for methane dehydroaromatization, are altered by directing the way...
journal article 2018
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Vollmer, I. (author), Yarulina, I. (author), Kapteijn, F. (author), Gascon, Jorge (author)
To secure future supply of aromatics, methane is a commercially interesting alternative feedstock. Direct conversion of methane into aromatics combines the challenge of activating one of the strongest C-H bonds in all hydrocarbons with the selective aromatization over zeolites. To address these challenges, smart catalyst and process design...
journal article 2018
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Shan, M. (author), Liu, X. (author), Wang, X. (author), Yarulina, I. (author), Seoane, Beatriz (author), Kapteijn, F. (author), Gascon, Jorge (author)
The development of new membranes with high H<sub>2</sub> separation performance under industrially relevant conditions (high temperatures and pressures) is of primary importance. For instance, these membranes may facilitate the implementation of energy-efficient precombustion CO<sub>2</sub> capture or reduce energy intensity in other...
journal article 2018
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Sabetghadam, A. (author), Liu, X. (author), Orsi, Angelica F. (author), Lozinska, Magdalena M. (author), Johnson, Timothy (author), Jansen, K.M.B. (author), Wright, Paul A. (author), Carta, Mariolino (author), McKeown, Neil B. (author), Kapteijn, F. (author), Gascon, Jorge (author)
Membrane separation for gas purification is an energy-efficient and environment-friendly technology. However, the development of high performance membranes is still a great challenge. In principle, mixed matrix membranes (MMMs) have the potential to overcome current materials limitations, but in practice there is no straightforward method to...
journal article 2018
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Benzaqui, Marvin (author), Pillai, Renjith S. (author), Sabetghadam, A. (author), Benoit, Virginie (author), Normand, Perine (author), Marrot, Jérôme (author), Menguy, Nicolas (author), Montero, David (author), Shepard, William (author), Tissot, Antoine (author), Martineau-Corcos, Charlotte (author), Sicard, Clémence (author), Mihaylov, Mihail (author), Carn, Florent (author), Beurroies, Isabelle (author), Llewellyn, Philip L. (author), De Weireld, Guy (author), Hadjiivanov, Konstantin (author), Gascon, Jorge (author), Kapteijn, F. (author), Maurin, Guillaume (author), Steunou, Nathalie (author), Serre, Christian (author)
A microporous Al trimesate-based metal-organic framework (MOF), denoted MIL-96-(Al), was selected as a porous hybrid filler for the processing of mixed matrix membranes (MMMs) for CO<sub>2</sub>/N<sub>2</sub> postcombustion separation. First, the structural model of MIL-96-(Al) initially reported was revisited using a combination of...
journal article 2017
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Osadchii, D. (author), Olivos Suarez, A.I. (author), Bavykina, A.V. (author), Gascon, Jorge (author)
Covalent triazine frameworks (CTFs) are porous organic materials promising for applications in catalysis and separation due to their high stability, adjustable porosity, and intrinsic nitrogen functionalities. CTFs are prepared by ionothermal trimerization of aromatic nitriles; however, multiple side reactions also occur under synthesis...
journal article 2017
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Sun, X. (author), Olivos Suarez, A.I. (author), Meijerink, Mark (author), Van Deelen, Tom (author), Ould-Chikh, Samy (author), Zečević, Jovana (author), de Jong, K.M. (author), Kapteijn, F. (author), Gascon, Jorge (author)
The development of synthetic protocols for the preparation of highly loaded metal nanoparticle-supported catalysts has received a great deal of attention over the last few decades. Independently controlling metal loading, nanoparticle size, distribution, and accessibility has proven challenging because of the clear interdependence between...
journal article 2017
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Oar-Arteta Gonzalez, L. (author), Valero Romero, M.J. (author), Wezendonk, T.A. (author), Kapteijn, F. (author), Gascon, Jorge (author)
High productivity towards C2–C4 olefins together with high catalyst stability are key for optimum operation in high temperature Fischer–Tropsch synthesis (HT-FTS). Here, we report the fabrication of Fe@C/Al composites that combine both the outstanding catalytic properties of the Fe–BTC MOF-derived Fe catalyst and the excellent mechanical...
journal article 2017
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Bavykina, A.V. (author), Olivos Suarez, A.I. (author), Osadchii, D. (author), Valecha, R.R. (author), Franz, R.P.M. (author), Makkee, M. (author), Kapteijn, F. (author), Gascon, Jorge (author)
A quasi chemical vapor deposition method for the manufacture of well-defined covalent triazine framework (CTF) coatings on cordierite monoliths is reported. The resulting supported porous organic polymer is an excellent support for the immobilization of two different homogeneous catalysts: (1) an Ir<sup>III</sup>Cp∗-based catalyst for the...
journal article 2017
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Sachdeva, S. (author), Koper, S.J.H. (author), Sabetghadam, A. (author), Soccol, Dimitri (author), Gravesteijn, Dirk J. (author), Kapteijn, F. (author), Sudhölter, Ernst J. R. (author), Gascon, Jorge (author), de Smet, L.C.P.M. (author)
Affinity layers play a crucial role in chemical sensors for the selective and sensitive detection of analytes. Here, we report the use of composite affinity layers containing Metal Organic Frameworks (MOFs) in a polymeric matrix for sensing purposes. Nanoparticles of NH<sub>2</sub>-MIL-53(Al) were dispersed in a Matrimid polymer matrix with...
journal article 2017
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Goetze, Joris (author), Meirer, Florian (author), Yarulina, I. (author), Gascon, Jorge (author), Kapteijn, F. (author), Ruiz-Martínez, Javier (author), Weckhuysen, Bert M. (author)
The nature and evolution of the hydrocarbon pool (HP) species during the Methanol-to-Olefins (MTO) process for three small-pore zeolite catalysts, with a different framework consisting of large cages interconnected by small eight-ring windows (CHA, DDR, and LEV) was studied at reaction temperatures between 350 and 450 °C using a combination...
journal article 2017
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Sun, X. (author), Olivos Suarez, A.I. (author), Oar-Arteta Gonzalez, L. (author), Rozhko, E. (author), Osadchii, D. (author), Bavykina, A.V. (author), Kapteijn, F. (author), Gascon, Jorge (author)
A Co@N-doped carbon (Co@ NC) hybrid was synthesized by thermal decomposition of the metal–organic framework (MOF) ZIF-67 under N2 atmosphere. These hybrid materials exhibit outstanding catalytic activity and chemoselectivity for the conversion of a wide range of substituted nitroarenes to their corresponding anilines under relatively mild...
journal article 2017
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