Cooperativity in Aqueous Organometallic Catalysis: Contribution of Cyclodextrin-Substituted Polymers
Jonathan PotierStéphane MenuelDavid FournierSophie FourmentinPatrice WoiselÉric MonflierFrédéric Hapiot
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Abstract:
Cooperativity has been implicated to explain the catalytic performances of cyclodextrin-substituted polymers in aqueous rhodium-catalyzed hydroformylation of 1-hexadecene, thus opening the door to the transformation of very hydrophobic substrates in aqueous biphasic catalysis by supramolecular means.Keywords:
Cooperativity
Supramolecular catalysis
Organometallic Chemistry
Cooperativity in Aqueous Organometallic Catalysis: Contribution of Cyclodextrin-Substituted Polymers
Cooperativity has been implicated to explain the catalytic performances of cyclodextrin-substituted polymers in aqueous rhodium-catalyzed hydroformylation of 1-hexadecene, thus opening the door to the transformation of very hydrophobic substrates in aqueous biphasic catalysis by supramolecular means.
Cooperativity
Supramolecular catalysis
Organometallic Chemistry
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Organometallic Chemistry
1-Hexene
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Abstract Transition metal ions are effective catalysts of the hydrolytic cleavage of amino acid esters and their effects can be enhanced and properly directed when they are chelated to functionalized ligands. The resulting metallocatalysts are attracting increasing attention and the systems so far investigated are briefly reviewed. Particular emphasis is given to supramolecular systems which may add to the metallocatalysts the benefits of the cooperativity, set upon convergent non‐covalent interactions of their components, needed for substrate recognition. The results obtained with metallomicellar aggregates and molecular metalloreceptors, with particular reference to those studied in the authors' laboratory, are reported in more detail. In the case of loosely structured metallomicelles, remarkable accelerations and, generally, modest selectivities have been observed; less spectacular kinetic effects, but promising substrate selectivity, have been obtained with structurally well defined metalloreceptors.
Cooperativity
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Aqueous medium
Molecular Recognition
Supramolecular catalysis
Calixarene
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Transition-metal-catalyzed hydroformylation has become an essential tool for the synthesis of aldehydes. In this paper, we highlight several examples of synthetically useful applications of homogeneous and heterogeneous rhodium-catalyzed hydroformylation, as well as several examples of tandem processes involving hydroformylation as a reaction step developed in our laboratory.
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Homogeneous Catalysis
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With new characteristics of cyclodextrin discovered and more derivatives of cyclodextrin synthesized,the applications of supramolecular cyclodextrin become more and more extensive.This paper summerized the research progress of supramolecular cyclodextrin in molecular recognition,molecular self-assembly and bio-enzyme mimics.And the development tendency of supramolecular cyclodextrin was prospected.
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Abstract The hydroformylation or oxo‐synthesis is one of the most important transition metal assisted homogeneous catalytic transformation, providing industrial‐scale production of aldehydes and alcohols. The hydroformylation—homogeneous article presents the basic chemistry and kinetics of hydroformylation, solvents of hydroformlylation, and side reactions accompanying hydroformylation. The detailed reaction mechanisms related to the cobalt‐ and rhodium‐modified and unmodified catalysts are presented as well. The chemistry of the individual steps of the classic catalytic cycle based on results of model reactions and spectroscopic investigations is discussed and is followed by an overview of different catalyst modifiers such as phosphine and phosphite ligands.
Homogeneous Catalysis
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A survey of protein databases indicates that the majority of enzymes exist in oligomeric forms, with about half of those found in the UniProt database being homodimeric. Understanding why many enzymes are in their dimeric form is imperative. Recent developments in experimental and computational techniques have allowed for a deeper comprehension of the cooperative interactions between the subunits of dimeric enzymes. This review aims to succinctly summarize these recent advancements by providing an overview of experimental and theoretical methods, as well as an understanding of cooperativity in substrate binding and the molecular mechanisms of cooperative catalysis within homodimeric enzymes. Focus is set upon the beneficial effects of dimerization and cooperative catalysis. These advancements not only provide essential case studies and theoretical support for comprehending dimeric enzyme catalysis but also serve as a foundation for designing highly efficient catalysts, such as dimeric organic catalysts. Moreover, these developments have significant implications for drug design, as exemplified by Paxlovid, which was designed for the homodimeric main protease of SARS-CoV-2.
Cooperativity
Supramolecular catalysis
Enzyme Catalysis
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