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HKUST Call Number: Thesis CHEM 2004 Leung.
Supramolecular Catalysis Provides a timely and detailed overview of the expanding field of supramolecular catalysis The subdiscpline of supramolecular catalysis has expanded in recent years, benefiting from the development of homogeneous catalysis and supramolecular chemistry. Supramolecular catalysis allows chemists to design custom-tailored metal and organic catalysts by devising non-covalent interactions between the various components of the reaction. Edited by two world-renowned researchers, Supramolecular Catalysis: New Directions and Developments summarizes the most significant developments in the dynamic, interdisciplinary field. Contributions from an international panel of more than forty experts address a broad range of topics covering both organic and metal catalysts, including emergent catalysis by self-replicating molecules, switchable catalysis using allosteric effects, supramolecular helical catalysts, and transition metal catalysis in confined spaces. This authoritative and up-to-date volume: Covers ligand-ligand interactions, assembled multi-component catalysts, ligand-substrate interactions, and supramolecular organocatalysis and non-classical interactions Presents recent work on supramolecular catalysis in water, supramolecular allosteric catalysis, and catalysis promoted by discrete cages, capsules, and other confined environments Highlights current research trends and discusses the future of supramolecular catalysis Includes full references and numerous figures, tables, and color illustrations Supramolecular Catalysis: New Directions and Developments is essential reading for catalytic chemists, complex chemists, biochemists, polymer chemists, spectroscopists, and chemists working with organometallics.
This book presents the latest synthetic protocols for the assembly of functionalized Cp ligands and their transition metal complexes. Cyclopentadienyl (Cp) complexes of transition metals belong to the most important classes of transition metal complexes with tightly bound ligands in the coordination sphere since their discovery in the middle of the last century. Even though they have been known for a long time, this field constantly evolves to deliver novel modified Cp ligands and complexes and to blossom into new fields of application. Beside the synthesis of ligands and metal complexes this book concentrates on novel and prospering fields of their application in organic synthesis. In this respect the Cp complexes have been applied to induce and catalyze various significant chemical transformations such as new C-C bond formation involving unsaturated substrates (e.g. cyclotrimerizations, cycloadditions, carbometallations, etc.), C-H bond and C-C bond activations followed by subsequent reactions (e.g. arylation, alkenylations, annulations, etc.), as well as many other processes. This volume also covers the recent development and application of chiral Cp complexes in enantioselective synthesis.
As the incorporation of more renewable electricity into the power-grid leads to surplus generation, methods to utilize electricity to drive chemical reactions are becoming more relevant. Immobilizaton of molecular electrocatalysts combines the mechanistic understanding of molecular catalysts with the advantages of heterogeneous catalysts. Electrocatalysts of the type Ni(P2N2)2 are well-understood molecular catalysts that can achieve enzyme-like activity for hydrogen evolution and oxidation in solution. This extraordinary performance is attributed to their unique structure with proton shuttles in the second coordination sphere. Previously this amine substituent was used for surface attachment to immobilize this catalyst onto electrodes. However, the mobility of this substituent is crucial to the activity of the catalyst. We evaluated possible synthetic pathways to incorporate surface attachable functionality on the phosphine substituent of these ligands. Due to the high reactivity of the phosphines involved in the synthesis, incorporation of surface attachable groups through established synthetic protocols was found to be not feasible. A synthesis based on post-synthetic modification of P[superscript ArBr]2N[superscript Ph]2 was identified as the best way to incorporate attachable surface groups. This strategy was subsequently utilized to synthesize complexes of the type Ni(P2N2)2 with unprecedented, highly functionalized, surface attachable phosphine substituents. Phosphonate modified ligands and their corresponding nickel complexes were isolated and characterized. Subsequent deprotection of the phosphonic ester derivatives provided the first Ni(P2N2)2 catalyst that can be covalently attached via pendent phosphonate groups to an electrode without the involvement of hte important pendent amine groups. Mesoporous TiO2 electrodes were surface modified by attachment of the new phosphonate functionalized complexes, and these provided electrocatalytic materials that proved to be competent and stable for sustained hydrogen evolution in aqueous solution at mild pH and low over potential. We directly compared the new ligand to a previously reported complex that utilized the amine moiety for surface attachment. Using HER as the benchmark reaction, the P-attached catalyst showed a marginally (9-14%) higher turnover frequency than its N-attached counterpart. Finally, we report the synthesis of three new iridium piano-stool complexes that are immobilized on gold surfaces through thiol groups. We characterized these molecules using surface-sensitive IR spectroscopy. Further studies with these molecules are geared towards promoting the non-faradaic electrochemical tuning of catalysts using interfacial electric fields.