Design of luminescent dinuclear platinum(II) complexes and iridium(III) catalytic hydrogen gas generation




Cinninger, Leander Michael

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The use of hydrogen gas as an alternative to a petroleum fuel source has become a primary focus in research in the last decade to decrease global greenhouse gas emissions. However, further improvements in the safe storage of hydrogen gas must be developed before it can become a viable alternative fuel source. One possibility is the use of the non-flammable solid, ammonia-borane, as a form of molecular hydrogen storage. Ammonia-borane can be readily dehydrogenated using transition metal catalysts to generate hydrogen gas. One such dehydrogenation catalyst is the iridium pincer complex, (1,3-OPt-Bu₂)₂C₆H₃)Ir(H)₂, which has been shown to readily react with substituted ammonia-borane to generate hydrogen gas by Heinekey and coworkers. Our focus is to functionalize the iridium catalyst, (1,3-OPt-Bu₂)₂C₆H₃)Ir(H)₂, with capped 3,4-ethylenedioxythiophene groups to determine if functionalization of the ligand with electropolymerizable groups will alter the catalytic activity. The transportation sector along with the production of electricity for lighting applications is estimated to generate 18% of the global greenhouse gas emissions. Thus, efficiency gains in the lighting sector along with alternative fuel sources for transportation would significantly cut the global greenhouse gas emissions. One potential way to more effectively use electricity for lighting applications is the development of more efficient solid-state lighting. One promising new form of solid-state lighting that is currently being developed are light-emitting electrochemical cells (LEECs). Herein is reported the synthesis, characterization, and study of the photophysical properties of a series of novel pyrazolate bridged dinuclear Pt(II) complexes. The incorporation of the 3,5-diphenylpyrazole bridged dinuclear Pt(II) complex into a light-emitting electrochemical cell is also discussed. In developing novel ligands and metal complexes, understanding the solid-state properties of these materials is of fundamental importance. One way in which this may be accomplished is through the use of x-ray crystallography. Single crystals of several novel organic ligands and metal complexes have been grown and their single crystal structures have been determined and fully analyzed for key crystallographic features.



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