| Catalysis is a technology of vital importance, enabling the production of many goods which are essential to the modern lifestyle. As such, the continued development of catalysis is of great importance, helping to reduce the costs and environment harm associated with the modern economy.;This thesis describes the study and design of pincer iridium complexes, a type of organometallic complex which can catalyze multiple reactions, including alkane dehydrogenation. If these catalysts are developed sufficiently, in the future they may have commercial applications for the production of fuels and commodity chemicals.;The research described in this thesis focused upon catalytic activity and selectivity, two aspects of a catalytic performance, for study and improvement. Understanding the steric and electronic properties which determine activity and selectivity, from a mechanistic viewpoint, should allowed for the rational and effective design of new, higher-performing catalysts.;First, the regioselectivity of dehydrogenation was examined through a combination of experimental and computational methods. The influence of each steric and electronic factor was both identified and quantified. Next, catalytic activity was investigated using a similar approach, showing that massive changes in activity (orders of magnitude) could be attributed to a single electronic factor.;With these mechanistic insights in hand, the rational design of new catalysts was begun. Computational studies suggested that cationic catalysts would be several hundred fold more active than their neutral counterparts, and synthetic progress was made in that direction.;Carefully considering the mechanism of dehydrogenation also allowed for process chemistry improvements which increased activity significantly. Lastly, the role of additives to dehydrogenation was also investigated, showing that certain Bronsted bases improved catalytic activity significantly. |
