Supramolecular catalysis. Part 2: artificial enzyme mimics

The design of artificial catalysts able to compete with the catalytic proficiency of enzymes is an intense subject of research. Non-covalent interactions are thought to be involved in several properties of enzymatic catalysis, notably (i) the confinement of the substrates and the active site within...

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Published inChemical Society reviews Vol. 43; no. 5; pp. 1734 - 1787
Main Authors Raynal, Matthieu, Ballester, Pablo, Vidal-Ferran, Anton, van Leeuwen, Piet W. N. M
Format Journal Article
LanguageEnglish
Published England Royal Society of Chemistry 07.03.2014
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Summary:The design of artificial catalysts able to compete with the catalytic proficiency of enzymes is an intense subject of research. Non-covalent interactions are thought to be involved in several properties of enzymatic catalysis, notably (i) the confinement of the substrates and the active site within a catalytic pocket, (ii) the creation of a hydrophobic pocket in water, (iii) self-replication properties and (iv) allosteric properties. The origins of the enhanced rates and high catalytic selectivities associated with these properties are still a matter of debate. Stabilisation of the transition state and favourable conformations of the active site and the product(s) are probably part of the answer. We present here artificial catalysts and biomacromolecule hybrid catalysts which constitute good models towards the development of truly competitive artificial enzymes. Supramolecular interactions were used for the design of catalytic enzyme mimics that possess one or more of the properties of enzymes. This review discusses successful examples of host-guest catalysts, catalysts operating in water, self-replicators, allosteric catalysts and biomacromolecule hybrid catalysts.
Bibliography:Piet van Leeuwen is a Group Leader at the ICIQ in Tarragona since April 2004. After completing his Thesis (Leyden University) in 1967, he worked with Shell Research Amsterdam for twenty six years. Since 1989, part-time, and since 1994, full time, he has initiated and led the homogeneous catalysis group at the University of Amsterdam. He held the chair of Industrial Homogeneous Catalysis at the Technical University of Eindhoven from 2001 till 2006. In 2005 he received the Holleman Prize from the Royal Netherlands Academy of Arts and Sciences. He was awarded a European Research Council Advanced Grant for his project "A New Vision on Nanocatalysts, NanosOnWings" in 2009. His interests range from fundamental aspects to applied catalysis utilizing mainly late transition metals with a focus on carbonylation catalysis. New areas to which he has contributed include supramolecular catalysis, dendrimer catalysis, effects of wide bite angles, and in situ spectroscopy.
Anton Vidal earned an undergraduate degree in Chemical Engineering at the Institut Químic de Sarrià (1987), where he completed his PhD on the synthesis of new heterocycles, with Prof. P. Victory (1992), followed by postdoctoral appointments at the University of Cambridge (Prof. J. K. M. Sanders, 1993-1994) and the University of Barcelona (Prof. M. A. Pericàs, 1995-1999). He gained industrial experience at Bayer-AG (Leverkusen, 1999 to 2003). Following the appointment as ICREA (Catalan Institution for Research and Advanced Studies) Research Professor, he started his independent research activities as a Group Leader at the Institute of Chemical Research of Catalonia (ICIQ) in Tarragona, Spain, in September 2003. He aims to design and develop efficient and sustainable catalytic tools for asymmetric synthesis, through a combination of modular design of the catalytic systems, the study of the molecular recognition processes that govern the catalytic event, and the use of computational methods.
Matthieu Raynal was born in Montauban, France, in 1982. He got his engineering diploma from ENSIACET (Toulouse) in 2005 and obtained his PhD degree under the supervision of Dr Pierre Braunstein (Université de Strasbourg) in 2009. He conducted postdoctoral studies at the Université Pierre et Marie Curie (Paris, France) and in the group of Prof. Piet W. N. M. van Leeuwen at the Institute of Chemical Research of Catalonia (ICIQ, Tarragona, Spain). In 2012, he was appointed as a CNRS researcher in the Laboratoire de Chimie des Polymères (UMR 7610) in the team of L. Bouteiller. His current research topics deal with the self-assembly properties of hydrogen-bonded supramolecular polymers, the prediction of organogel formation using the Hansen solubility parameters and the design of supramolecular catalysts.
Pablo Ballester was born in 1959 in Palma de Mallorca, Spain. He studied Chemistry at the University of the Balearic Islands (UIB) where he also completed the PhD degree in 1986 under the direction of Prof. Ramón Mestres. He worked as a postdoctoral fellow with Prof. Julius Rebek Jr at the University of Pittsburgh and MIT for three years and for one year at the UIB with Prof. José M. Saá. In 1990 he joined the Chemistry Department of UIB where he held the positions of Assistant and Associate Professor. In 2004 he was awarded with an ICREA Research Professorship and moved to the Institute of Chemical Research of Catalonia (ICIQ) to become a group leader. His current research interests are in the areas of molecular self-assembly, molecular recognition and supramolecular catalysis.
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ISSN:0306-0012
1460-4744
1460-4744
DOI:10.1039/c3cs60037h