Emiel J. M. Hensen

Eindhoven University of Technology

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Evgeny A. Pidko

Delft University of Technology

147

Rutger A. van Santen

Eindhoven University of Technology

116

Nikolay Kosinov

Eindhoven University of Technology

Ivo A. W. Filot

Eindhoven University of Technology

Jan P. Hofmann

Eindhoven University of Technology

Brahim Mezari

Eindhoven University of Technology

Yaqiong Su

Xi'an Jiaotong University

Michael D. Boot

Eindhoven University of Technology

Alexander Parastaev

Eindhoven University of Technology

Evgeny A. Uslamin

Delft University of Technology

Cooperative Institutions

Eindhoven University of Technology

375

Utrecht University

131

Institute of Catalysis and Petrochemistry

121

Chinese Academy of Sciences

108

Delft University of Technology

Centre National de la Recherche Scientifique

University of Chinese Academy of Sciences

KU Leuven

University of Groningen

ETH Zurich

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Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol

Nature Communications (2015)

Sebastian Grundner Monica A. C. Markovits Guanna Li Moniek Tromp Evgeny A. Pidko

Abstract Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.

Methane Monooxygenase

Mordenite

Reactivity

10.1038/ncomms8546

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Citations (701)

Aqueous phase reforming of glycerol over Re-promoted Pt and Rh catalysts

Green Chemistry (2013)

Ayşegül Çiftçi D. A. J. Michel Ligthart Emiel J. M. Hensen

The potential of Re promotion for carbon-supported Pt and Rh nanoparticles was investigated for aqueous phase reforming (APR) of glycerol as a model compound for biobased feedstock. Upon alloying with Re, the overall conversion rate of glycerol was substantially increased for both metal catalysts. Whereas Pt/C is more active than Rh/C in glycerol APR, the RhRe/C catalyst outperforms PtRe/C. The overall APR catalytic performance strongly correlates with the activity trend for the gas-phase water–gas shift (WGS) reaction. RhRe/C exhibited the highest activity in APR and WGS reactions. A very strong synergy between Rh and Re and Pt and Re is observed in the model WGS reaction. The role of Re in the bimetallic catalysts is to facilitate water dissociation, effectively increasing the WGS activity. During APR, this results in lower steady-state CO coverage and increased glycerol conversion rates. In terms of selectivity, the yield of renewable hydrogen is increased. The use of Re as a promoter also results in significant changes in the product selectivities during glycerol APR. Although gas-phase acetaldehyde decomposition measurements evidenced that alloying with Re increased C–C bond cleavage activities of Pt/C and Rh/C, the increased acidity due to acidic hydroxyl groups bound to Re resulted in a more substantial increase of dehydration reactions. Whereas Rh/C is more selective for formation of products involving C–C bond cleavage than Pt/C, the product mixtures of their alloys with Re reflect a much increased ratio of C–O vs. C–C bond cleavage reaction rates.

Bimetallic strip

Bond cleavage

Water-gas shift reaction

Hydrogenolysis

10.1039/c3gc42046a

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Citations (77)

Mesoporous SSZ-13 zeolite prepared by a dual-template method with improved performance in the methanol-to-olefins reaction

Journal of Catalysis (2012)

Leilei Wu Volkan Degirmenci Pieter C. M. M. Magusin Nick J.H.G.M. Lousberg Emiel J. M. Hensen

Chabazite

Space velocity

Ammonium hydroxide

10.1016/j.jcat.2012.10.029

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Citations (158)

The catalytic performance of Cu-containing zeolites in N2O decomposition and the influence of O2, NO and H2O on recombination of oxygen

Journal of Catalysis (2008)

P SMEETS Bert F. Sels R VANTEEFFELEN Hugo Leeman Emiel J. M. Hensen

Oxygen evolution

10.1016/j.jcat.2008.03.008

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Citations (104)

One-Step Synthesis of Hierarchical ZSM-5 Using Cetyltrimethylammonium as Mesoporogen and Structure-Directing Agent

Chemistry of Materials (2017)

Lingqian Meng Brahim Mezari Maarten G. Goesten Emiel J. M. Hensen

Hierarchical ZSM-5 zeolite is hydrothermally synthesized in a single step with cetyltrimethylammonium (CTA) hydroxide acting as mesoporogen and structure-directing agent. Essential to this synthesis is the replacement of NaOH with KOH. An in-depth solid-state NMR study reveals that, after early electrostatic interaction between condensed silica and the head group of CTA, ZSM-5 crystallizes around the structure-directing agent. The crucial aspect of using KOH instead of NaOH lies in the faster dissolution of silica, thereby providing sufficient nutrients for zeolite nucleation. The hierarchical ZSM-5 zeolite contains mesopores and shows excellent catalytic performance in the methanol-to-hydrocarbons reaction.

ZSM-5

10.1021/acs.chemmater.7b00913

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Citations (99)

Manganese as a structural promoter in silica-supported cobalt Fischer-Tropsch catalysts under simulated high conversion conditions

Journal of Catalysis (2023)

Luke M. van Koppen A. Iulian Dugulan G. Leendert Bezemer Emiel J. M. Hensen

Understanding the deactivation mechanism of cobalt-based Fischer-Tropsch catalysts is of significant practical importance. Herein, we explored the role of manganese as a structural promoter on silica-supported cobalt nanoparticles under simulated high CO conversion conditions, i.e., high relative humidity. The structural changes in cobalt dispersion and oxidation state were followed by in situ Mössbauer emission spectroscopy. Adding manganese oxide to silica-supported cobalt enhanced the dispersion of metallic cobalt in the reduced catalysts. This higher cobalt dispersion, however, led to a stronger tendency of cobalt silicate formation under humid conditions. Without manganese, the cobalt particles sintered, and the larger ones were prone to transformation into cobalt carbide under high conversion conditions. As such, silica is not preferred as a support for practical FTS.

Fischer–Tropsch process

Cobalt oxide

10.1016/j.jcat.2023.115173

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Citations (2)

CCDC 948171: Experimental Crystal Structure Determination

The Cambridge Structural Database (2016)

Georgy A. Filonenko Matthew P. Conley Christophe Copéret Martin Lutz Emiel J. M. Hensen

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

10.5517/ccdc.csd.cc10tn5n

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Citations (0)

CCDC 972638: Experimental Crystal Structure Determination

The Cambridge Structural Database (2016)

Georgy A. Filonenko Elena Cosimi Laurent Lefort Matthew P. Conley Christophe Copéret

10.5517/ccdc.csd.cc11n3f7

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Strong Ni-MnO Synergy in the Sabatier Reaction

12th Natural Gas Conversion Symposium (2019)

Emiel J. M. Hensen Wilbert L. Vrijburg

Source

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Nitrate electrochemical reduction to ammonia on Cu2O catalysts

Dimitra Anastasiadou Yvette van Beek Wei Chen Tim Wissink Alexander Parastaev

This manuscript reports the electrosynthesis of ammonia from nitrate catalysed by Cu2O. Cu2O (111) and (100) preferential orientations were prepared through electrodeposition to investigate the effect of surface structure. Cu2O (111) is more active and selective for ammonia formation than Cu2O (100). The highest faradaic efficiency (FE) was achieved for both catalysts at -0.3 V vs RHE, with Cu2O (111) reaching up to 80%. Additional measurements with quasi-in situ X-ray photoelectron spectroscopy and in-situ Raman spectroscopy revealed that Cu0 is the active phase during the reaction. The stability of the catalysts was examined by ex-situ methods such as scanning electron microscopy, X-ray diffraction and inductively coupled plasma-optical emission spectrometry. The catalysts undergo severe morphological changes as a function of the applied potential and the reaction time, most likely due to the dissolution and redeposition of Cu. After three hours of reaction, the entire surface of the catalysts was reconstructed into nanoneedles. The final FE was still higher for the original Cu2O (111) electrode.

Electrosynthesis

Ammonia production

10.26434/chemrxiv-2022-w6vr8

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Citations (1)