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EXPLORING NEW ASYMMETRIC REACTIONS CATALYSED by DICATIONIC Pd(II) COMPLEXES

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EXPLORING NEW ASYMMETRIC REACTIONS CATALYSED by DICATIONIC Pd(II) COMPLEXES EXPLORING NEW ASYMMETRIC REACTIONS CATALYSED BY DICATIONIC Pd(II) COMPLEXES A DISSERTATION FOR THE DEGREE OF DOCTOR OF PHILOSOPHY FROM IMPERIAL COLLEGE LONDON BY ALEXANDER SMITH MAY 2010 DEPARTMENT OF CHEMISTRY IMPERIAL COLLEGE LONDON DECLARATION I confirm that this report is my own work and where reference is made to other research this is referenced in text. ……………………………………………………………………… Copyright Notice Imperial College of Science, Technology and Medicine Department Of Chemistry Exploring new asymmetric reactions catalysed by dicationic Pd(II) complexes © 2010 Alexander Smith [email protected] This publication may be distributed freely in its entirety and in its original form without the consent of the copyright owner. Use of this material in any other published works must be appropriately referenced, and, if necessary, permission sought from the copyright owner. Published by: Alexander Smith Department of Chemistry Imperial College London South Kensington campus, London, SW7 2AZ UK www.imperial.ac.uk ACKNOWLEDGEMENTS I wish to thank my supervisor, Dr Mimi Hii, for her support throughout my PhD, without which this project could not have existed. Mimi’s passion for research and boundless optimism have been crucial, turning failures into learning curves, and ultimately leading this project to success. She has always been able to spare the time to advise me and provide fresh ideas, and I am grateful for this patience, generosity and support. In addition, Mimi’s open-minded and multi-disciplinary approach to chemistry has allowed the project to develop in new and unexpected directions, and has fundamentally changed my attitude to chemistry. I would like to express my gratitude to Dr Denis Billen from Pfizer, who also provided a much needed dose of optimism and enthusiasm in the early stages of the project, and managed to arrange my three month placement at Pfizer despite moving to the US as the department closed. It would have been easy on his part to cancel the visit under these circumstances and I am grateful for his efforts in allowing me the opportunity to work in his lab. Denis’ regular visits have been missed since the move, and I would also like to give thanks for his continued interest in the project and my thesis. I have also had the opportunity to work closely with Prof Henry Rzepa whose ongoing efforts have saved us from an intractable problem with the project. His results revealed an unanticipated level of complexity in our system, enhancing the significance of our findings, and I am very grateful for his contributions. Thanks goes to all members, past and present, of the KKH group for their friendship and assistance. In particular I would like to name Andrewie, Emma and Jason, who welcomed me to the group and provided support when I first arrived, as well as Luis, Xinzhu, Jannine, Laura, Natalia, Bao, Silvia and Steven who continue to make the KKH group a sociable, stimulating and productive place to work. Outside of the lab we have had some great times, whether it be a conference in Florence or a night in Reflex, and I’m looking forward to more KKH socials in the future. i Thanks also to Tony, Oliver and all the other employees I had the pleasure to work with at Cancer Research Technology, who gave me the passion to pursue a career in medicinal chemistry. Special thanks goes to my girlfriend, Charlotte. As long as I have had her love and reassurance, every problem I have faced has been overcome, however I still remain cynical, every time, until she is proven right. I would also like to thank a wealth of other friends who supported me before and during my PhD. Of my friends from St Albans, some of who I have known for over 20 years, I would particularly like to thank James, as without his advice and assistance I may never have begun a career in this field. I am also grateful for the friendship of the people I have met in Nottingham and London who have made life all the more enjoyable. ii ABSTRACT Dicationic palladium(II) complexes have been shown to catalyse a number of important asymmetric transformations including Michael, Mannich and aldol reactions. This PhD thesis describes work undertaken to discover and develop novel applications of dicationic palladium(II) complexes in asymmetric catalysis. The introductory chapter outlines the advances in catalytic asymmetric α-functionlisation of β-ketoesters. This includes both metal-catalysed and organocatalytic processes with reference to C-C, C-X (X = F, Cl, Br), C-N, C-O and C-S bond forming reactions. Chapter 2 discusses the work towards the synthesis of β-amino acids via Michael reactions catalysed by Pd(II) complexes. These reactions failed to proceed with good enantioselectivities, leading to the investigation of a number of related transformations. In the following Chapter the reaction of β-ketoesters with oxaziridines to generate α- hydroxy-β-ketoesters was discovered. Extensive screening of reaction parameters led to the identification of dimethyldioxirane (DMD) as a superior oxidant for this reaction, providing ee’s of up to 98%. Examining a range of substrates revealed several key structural elements required for both reactivity and enantioselectivity. Determination of the absolute stereochemistry of the products revealed opposite facial selectivity to that reported in a number of related reactions. Chapter 4 discusses the results of DFT calculations undertaken by a colleague (Prof H. S. Rzepa), to identify the origins of stereoselectivity in the Pd(II) mediated α-hydroxylation of β-ketoesters with DMD. Chapter 5 discusses the investigation of carboxylated pyrrolidinones and succinimides as substrates in the hydroxylation reaction. Successful α-hydroxylation provided access to 3 classes of synthetically useful hydroxylated N-heterocyclic products with high optical purity, and brief synthetic studies directed towards the natural product Pramanicin were undertaken. The last Chapter contains experimental procedures and characterisation data of all the compounds synthesised during the course of this project. iii TABLE OF CONTENTS Acknowledgements ........................................................................................................... i Abstract ............................................................................................................................ iii Table of Contents ............................................................................................................ iv Abbreviations ................................................................................................................. vii Chapter 1: Introduction ......................................................................... 1 1.1. Catalytic Asymmetric α-Functionalisation of β-Ketoesters ......................... 1 1.1.1. Lewis Acid-Catalysed Methods................................................................ 3 1.1.1.1. Michael Reactions ................................................................................ 3 1.1.1.2. Other C-C Bond Forming Reactions .................................................. 16 1.1.1.3. C-Halogen Bond forming reactions .................................................... 19 1.1.1.4. C-N Bond Forming Reactions ............................................................ 24 1.1.1.5. C-S Bond Forming Reactions ............................................................. 26 1.1.1.6. C-O Bond Forming Reactions ............................................................ 27 1.1.2. Organocatalysis and Phase-transfer Catalysis ........................................ 29 1.1.2.1. Michael Reactions .............................................................................. 30 1.1.2.2. Other C-C Bond Forming Reactions .................................................. 35 1.1.2.3. C–Heteroatom Bond Forming Reactions ........................................... 39 1.2. Aims ........................................................................................................... 43 Chapter 2: Reactivity of Dicationic Pd(II) Triflates ......................... 45 2.1. Studies Towards γ-Amino Acids ................................................................ 45 2.1.1. Catalyst Preparation ................................................................................ 45 2.1.2. Synthesis of γ-Amino Acids ................................................................... 47 2.1.3. Nitroalkane – Michael Acceptor Approach ............................................ 50 2.1.3.1. Synthesis of precursors ....................................................................... 50 2.1.3.2. Michael Additions .............................................................................. 53 2.1.4. Nitroalkene – Michael Donor Approach ................................................ 62 2.1.4.1. Synthesis of Precursors ....................................................................... 62 2.1.4.2. Michael Additions .............................................................................. 63 iv 2.1.5. Other Michael Additions ........................................................................ 71 2.2. Wider Investigation of Palladium(II)-Catalysed Reactions........................ 73 2.2.1. Synthesis of Precursors ........................................................................... 73 2.2.2. Additions to Enol Ethers ........................................................................ 74 2.2.3. Additions to Aromatic Compounds ........................................................ 74 2.2.4.
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