Author Archive

HOT Article: “self-dosing” catalysts

Compared to homogeneous catalysts, heterogeneous catalysts used in hydrosilylation reactions are quite rare. In this HOT article, the catalytic activity and recyclability of PtO2 is examined for the hydrosilylation of n-octene with heptamethyltrisiloxane.

Compared to the usual homogeneous catalysts PtO2 dissolves only to a small degree after reaction with silane. The un-reacted solid catalyst is then easily separated from the reaction mixture by simple decantation or filtration and so can be used for subsequent runs. The observation of an induction period in every cycle indicates that the active species is formed in situ before the reaction can take place and new material has to dissolve for each run.

The active species is formed by reduction of PtO2 with the silane and is soluble in the reaction mixture. The solubility behavior together with the high activity allows a ‘‘self-dosing’’ of the catalyst—leading to little waste of precious metal in contrast to other ‘‘homogeneous’’ (i.e. better soluble) Pt-based catalysts making it potentially useful for industrial applications.

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PtO2 as a “self-dosing” hydrosilylation catalyst
Sophie Putzien, Eckhart Louis, Oskar Nuyken and Fritz E. Kühn
Catal. Sci. Technol., 2012, Advance Article
DOI: 10.1039/C2CY00367H

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HOT Article: Digestion produces high surface area catalysts

In this Catalysis Science and Technology HOT Article, the selective synthesis of an amorphous titania-zirconia mixed oxide with a very high specific surface area is described. The synthesized mixed oxide has been thoroughly characterized by various techniques and evaluated for an important oxidative dehrogenation reaction using CO2 as a soft oxidant.

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High surface area TiO2–Zr2 prepared by caustic solution treatment, and its catalytic efficiency in the oxidehydrogenation of para-ethyltoluene by CO2
Abhishek Burri, Nanzhe Jiang and Sang-Eon Park
Catal. Sci. Technol., 2012, Advance Article
DOI: 10.1039/C1CY00281C

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PERSPECTIVE: Imidazolium-derived organosilicas for catalysis

This perspective focuses on the catalytic uses of imidazolium derivatives grafted on to silicas, including metal catalysts (complexes and nanoparticles) and metal-free ones.  It is intended to help in inspiring future developments and interest in the growing field of catalysis by supported imidazolium salts and NHC (N-heterocyclic carbenes) complexes based on organosilicas.

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Imidazolium-derived organosilicas for catalytic applications
Amàlia Monge-Marcet, Roser Pleixats, Xavier Cattoën and Michel Wong Chi Man
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C1CY00287B

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HOT Article: Nanoparticle catalysis with the Midas touch

In this HOT article, the efforts of Graham Hutchings and co-workers to produce efficient catalysts based on gold and gold palladium nanoparticles supported on a variety of supports for the clean transformation of 1,2-propanediol (important in the synthesis of fine chemicals) to methyl lactate and methyl pyruvate are described.

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Oxidative esterification of 1,2-propanediol using gold and gold-palladium supported nanoparticles
Gemma L. Brett, Peter J. Miedziak, Nikolaos Dimitratos, Jose A. Lopez-Sanchez, Nicholas F. Dummer, Ramchandra Tiruvalam, Christopher J. Kiely, David W. Knight, Stuart H. Taylor, David J. Morgan, Albert F. Carley and Graham J. Hutchings
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C1CY00254F

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HOT Article: The role of carbide surface morphology on olefin metathesis reactivity

An increased industrial demand for propene, and potential applications in the processing of renewable raw materials has led to a strong renewal of interest in development of
heterogeneous olefin metathesis catalysis. Olefin metathesis proceeds through the formation of metal carbene initiating and propagating species. On contact with the reactant, catalyst precursors generate metal carbene initiating sites.  Active polycrystalline molybdenum carbide foils may be prepared through carbonyl bond breaking in chemisorbed aldehydes and ketones to yield surface alkylidene and oxo groups.  In this HOT article, helium ion microscopy imaging is used to characterize the foil as a first step towards determining if the carbide structure plays an important role in the olefin metathesis related surface chemistry.

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Spectroscopic and structural characterization of the formation of olefin metathesis initiating sites on unsupported ß-Mo2C
I. Temprano, G. Goubert, G. Behan, H. Zhang and P. H. McBreen
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C1CY00180A

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HOT article: Thermoregulation by cyclodextrins

This HOT article represents the first example of thermoregulation of the surface activity of an amphiphilic phosphane by a cyclodextrin.  This allows good activities at temperatures >100 ºC and good separations at 80 ºC and has the potential to be applied to other processes.

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Supramolecularly controlled surface activity of an amphiphilic ligand. Application to aqueous biphasic hydroformylation of higher olefins
Natacha Six, Antonella Guerriero, David Landy, Maurizio Peruzzini, Luca Gonsalvi, Frédéric Hapiot and Eric Monflier
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C1CY00156F

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PERSPECTIVE: Positive cooperativity and enhanced selectivity

In this Catalysis Science & Technology PERSPECTIVE, David Glueck examines several examples of structure–selectivity relationships with the eventual goal of designing substrates for positive cooperativity and enhanced selectivity in asymmetric catalysis.   This kind of systematic investigation hopefully is the way forward to rationally improve selectivity.

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Selectivity via catalyst or substrate control in catalytic asymmetric transformations of bifunctional symmetrical substrates
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C1CY00048A, Perspective

Designing substrates

Designing substrates for positive cooperativity and enhanced selectivity in asymmetric catalysis

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Hot Article: New cleaner catalysts for haloamines

New cleaner catalysts for haloamines

Mark Keane and co-workers have identified the  intermediates in beta-Mo nitride synthesis and report the first application of this nitride in the catalytic hydrogenation of nitroarenes.
The selective hydrogenation of p-chloronitrobenzene (p-CNB) to p-chloroaniline (p-CAN) has been used as a model reaction.

The authors hope that their findings may serve as the basis for the development of Mo2N materials as new catalysts for the cleaner production of commercially important aromatic amines with multiple applications in the fine chemical industry.

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Beta-Molybdenum nitride: synthesis mechanism and catalytic response in the gas phase hydrogenation of p-chloronitrobenzene
Fernando Cárdenas-Lizana, Santiago Gómez-Quero, Noémie Perret, Lioubov Kiwi-Minsker and Mark A. Keane
Catal. Sci. Technol., 2011, Advance Article

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PERSPECTIVE: Near size zero attained

Near size-zero attained

This PERSPECTIVE discuses the fundamentals and factors influencing the removal of the least reactive sterically hindered S-containing compounds present in transportation fuels, and more specifically in the diesel fraction.  Special attention is paid to the progress made in alternative process concepts and technologies that are being developed for ultra low sulfur fuels.

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Towards near zero-sulfur liquid fuels: a perspective review
Barbara Pawelec, Rufino M. Navarro, José Miguel Campos-Martin and José L. G. Fierro
Catal. Sci. Technol., 2011, Advance Article
DOI: 10.1039/C0CY00049C

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PERSPECTIVE: Two-dimensional zeolites: dream or reality?

Zeolite synthesis, has been vigorously explored and developed for more than half a century and yet most zeolites known to date have not been synthesized without templating with an appropriate organic molecule. But the discovery of zeolite MCM-22 promises to change all that. The MCM-22 framework was found to form by two pathways and unlike conventional 3D zeolites the layered precursor could be structurally modified after synthesis. With 2D zeolites adsorption and catalysis occur almost exclusively on the surface of these materials and not inside the zeolite pores as in conventional zeolites.
This PERSPECTIVE aims to provide an up-to-date knowledge and challenges associated with “two-dimensional zeolites (2D zeolites)”.

Two-dimensional zeolites

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Wieslaw J. Roth and Jiří Čejka, Catal.  Sci. Technol., 2011, Advance Article DOI: 10.1039/C0CY00027B, Perspective

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