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The objective of this thesis is to examine the photophysical and structural properties of Ru(II)/Re(I) based bimetallic complexes based on p-[N-2-(2’-pyridyl)benzimidazolyl]-[N-2-(2’-pyridyl)indolyl]-benzene (L1) ligand, as well as the photophysical and photochemical properties of N^C-chelate 4-coordinate organoboron compounds that contain a metal acetylide group. Ligand L1 was synthesized and fully characterized. Due to the incorporation of two distinct chelating sites, an N^N-chelate site and an N^C-chelate site, L1 has been found to be very effective in selective binding to two different metal ions. Two new heterobimetallic complexes Ru(II)-Pt(II) and Ru(II)-Pd(II) using L1 as the bridging ligand were prepared and fully characterized. All Ru(II)-containing complexes have been found to be luminescent. The Pt(II) unit appears to enhance phosphorescent efficiency of the Ru(II) unit while the Pd(II) unit has little influence. Using L1 as the bridging unit, two new Re(I) based heterobimetallic complexes Re(I)-Pt(II) and Re(I)-Pd(II) were also successfully synthesized. Results indicate that there is communication between the two different metal centers. The preliminary results indicated that the mononuclear Re(I) complex based on L1 is a promising candidate for the electrocatalytic CO2 reduction. Pd(II) and Pt(II) complexes were synthesized with an atropisomeric bis-pyridyl chelate ligand bis{3,3’-[N-Ph-2-(2’-py) indolyl]} (L4). To examine the potential use of the trans-chelate L4 ligand in oxidative coupling reactions catalyzed by Pd(II) compounds, acetoxylation of arenes by PhI(OAc)2 using PhI(OAc)2/L4 (2:1) as the catalyst was examined and found to accelerate the reaction, but lower the overall yield. Finally, to examine the impact of metal ions on photochromic properties of N^C-chelate organoboron compounds, three metal acetylide compounds that contain a photo-active N^C-chelate BMes2 unit (B(ppy)Mes2) were prepared and fully characterized. The studies indicated that by taking advantage of different heavy metals the photoisomerization quantum efficiency of the boron chromophores can be readily tuned through the adjustment of 3LC state localized on the chelate backbone or the involvement of MLCT state in the lowest energy electronic transition. / Thesis (Ph.D, Chemistry) -- Queen's University, 2013-01-07 15:20:45.675

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M.Sc. (Chemistry) / Please refer to full text to view abstract

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by Tung Suet Lam. / Thesis (M.Phil.)--Chinese University of Hong Kong, 2002. / Includes bibliographical references. / Abstracts in English and Chinese. / Table of Contents --- p.i / Acknowledgments --- p.iv / Abstract --- p.v / Abstract (Chinese version) --- p.vii / Abbreviations --- p.ix / List of Compounds --- p.xi / Chapter Chapter1. --- synthesis and structures of iron(ii) and cobalt(ii) complexes derived from pyridine-functionalized amido ligands / Chapter 1.1 --- INTRODUCTION --- p.1 / Chapter 1.1.1 --- General Background --- p.1 / Chapter 1.1.2 --- A Brief Review on Amides of the Late Transition Metals --- p.3 / Chapter 1.2 --- OBJECTIVES OF THIS WORK --- p.5 / Chapter 1.3 --- RESULTS AND DISCUSSION --- p.7 / Chapter 1.3.1 --- Alkali Metal Derivatives of N-Silylated 2-Aminopyridines --- p.7 / Chapter 1.3.1.a. --- "Synthesis of Aminopyridines [HN(SiMe3)》(2-C5H3N-6-R)] (R=H (1a), Me (1b)) and Their Lithium Derivatives" --- p.7 / Chapter 1.3.1.b. --- Synthesis of the Potassium Derivative [{K(L1)(tmeda)}2 ] (4) --- p.8 / Chapter 1.3.1.c. --- "Physical Characterization of Compounds 2a, 3 and" --- p.4 9 / Chapter 1.3.1.d. --- Molecular Structures of Compounds 3 and4 --- p.10 / Chapter 1.3.2 --- "Synthesis, Structures and Reactivities of Iron(II) and Cobalt(II) Amides" --- p.16 / Chapter 1.3.2.a. --- Synthesis of Mononuclear Iron(II) and Cobalt(II) Diamides --- p.16 / Chapter 1.3.2.b. --- Physical Characterization of Compounds 5-8 --- p.16 / Chapter 1.3.2.C. --- Molecular Structures of Compounds 5-8 --- p.17 / Chapter 1.4 --- EXPERIMENTAL FOR CHAPTER1 --- p.28 / Chapter 1.5 --- REFERENCES FOR CHAPTER1 --- p.31 / Chapter Chapter2. --- reaction of iron(II) and cobalt(II) amides with phenolic compounds / Chapter 2.1 --- "SYTHESIS, STRUCTURES AND REACTIVITIES OF IRON(II) AND COBALT(II) BIS(ARYLOXIDE)" --- p.36 / Chapter 2.1.a. --- "Reaction of Compounds 7 and 8 with 2,2 -ethylidenebis(4,6-di-tert-butyl phenol)" --- p.36 / Chapter 2.1.b. --- "Molecular Structures, Magnetic Moments, and Reactivities of Compounds 9and10" --- p.36 / Chapter 2.2 --- A GENERAL REVIEW ON CATECHOL DIOXYGENASES --- p.44 / Chapter 2.3 --- "SYTHESIS, STRUCTURES AND REACTIVITIES OF IRON(II) AND COBALT(II) CATECHOLATES" --- p.46 / Chapter 2.3.a. --- Synthesis of Binuclear Iron(II) and Cobalt(II) Catecholates --- p.46 / Chapter 2.3.b. --- Molecular Structures of Compounds 11 and12 --- p.48 / Chapter 2.3.c. --- Reactions of Compounds 11 and 12 with Dioxygen --- p.54 / Chapter 2.3.d. --- Identification of Oxidative Cleavage Products --- p.54 / Chapter 2.4 --- EXPERIMENTAL FOR CHAPTER2 --- p.56 / Chapter 2.5 --- REFERENCES FOR CHAPTER2 --- p.59 / Chapter Chapter3. --- synthesis of late transition metal amidinates / Chapter 3.1 --- INTRODUCTION --- p.62 / Chapter 3.1.1 --- General background --- p.62 / Chapter 3.1.1.a --- Metal´ؤAmidine Bonding Modes --- p.63 / Chapter 3.1.1.b. --- Preparation of Metal Amidinates Complexes --- p.64 / Chapter 3.1.2 --- "N-Silylated Benzamidinates of Li, Na and K 一 The Starting Materials" --- p.65 / Chapter 3.1.3 --- A General Review on The Chemistry of Low-Valent Late Transition- Metal Amidinates --- p.67 / Chapter 3.2 --- OBJECTIVES OF THIS WORK --- p.72 / Chapter 3.3 --- RESULTS AND DISCUSSION --- p.73 / Chapter 3.3.1 --- Synthesis and Structures of Lithium Benzamidinates --- p.73 / Chapter 3.3.1.a. --- "Synthesis of [Li(L3)(tmeda)] (L3 = [PhC(NSiMe3){N(2,6´ؤ Me2C6H3}]) and [Li(L4)(tmeda)] (L4 = [PyC(NSiMe3){N(2,6- Me2C6H3)}]) as Ligand´ؤTransfer Reagents" --- p.73 / Chapter 3.3.1.b. --- Physical Characterization of Compounds 15 and16 --- p.74 / Chapter 3.3.1.c. --- Molecular Structures of Compounds 15 and16 --- p.75 / Chapter 3.3.2 --- "Synthesis, Structures and Reactivities of Iron(II) and Cobalt(II) Amidinates" --- p.81 / Chapter 3.3.2.a. --- Synthesis of Mononuclear Iron(II) Benzamidinates --- p.81 / Chapter 3.3.2.b. --- Synthesis of a Binuclear Cobalt(II) Benzamidinate --- p.82 / Chapter 3.3.2.c. --- Physical Characterization of Compounds 17-19 --- p.83 / Chapter 3.3.2.d. --- Molecular Structures of Compounds 17-19 --- p.84 / Chapter 3.3.2.e. --- Reaction of Compound 18 with Dioxygen --- p.94 / Chapter 3.3.2.f. --- Molecular Structure of Compound20 --- p.95 / Chapter 3.3.3 --- Synthesis and Structures of Nickel(II) and Copper(I) Benzamidinates --- p.98 / Chapter 3.3.3.a --- Synthesis of a Nickel(II) Benzamidinate --- p.98 / Chapter 3.3.3.b. --- Synthesis of a Binuclear Copper(I) Benzamidinate --- p.99 / Chapter 3.3.3.c. --- Physical Characterization of Compounds 21 and22 --- p.101 / Chapter 3.3.3.d. --- Molecular Structures of Compounds 21 and22 --- p.102 / Chapter 3.3.4 --- Synthesis and Structures of Mononuclear Zinc(II) and Cadmium(II) Amidinates --- p.107 / Chapter 3.3.4.a --- Synthesis of Mononuclear Zinc(II) and Cadmium(II) Benzamidinates --- p.107 / Chapter 3.3.4.b. --- Physical Characterization of Compounds 23 and24 --- p.107 / Chapter 3.3.4.C. --- Molecular Structures of Compounds 23 and24 --- p.108 / Chapter 3.4 --- EXPERIMENTAL FOR CHAPTER3 --- p.113 / Chapter 3.5 --- REFERENCES FOR CHAPTER3 --- p.119 / appendix1 --- p.127 / appendix2 --- p.129