Over the last century, in the field of coordination chemistry, the number of template reactions has expanded into a diverse collection which can produce a variety of compounds. These template reactions have been used to afford compounds that would be difficult to obtain otherwise. One of the most famous template reactions is the synthesis of phthalocyanine, which was investigated by Linstead. After exploring the chemistry of phthalocyanine, Linstead synthesized hemiporphyrazines and bis(2-iminopyridyl)isoindolines from 1,3-diiminoisoindoline and various primary amines. Later, Siegl improved the synthesis of the hemiporphyrazines and the bis(2-iminopyridyl)isoindolines by employing a calcium ion as a templating agent. The template formation of isoindoline based macrocyclic compounds has been explored, however, the template formation of isoindoline based chelates is relatively unexplored. Due to its restrictive facial arrangement of carbonyl ligands and propensity to coordinate nitrogenous bases, the Re(CO) 3-unit is a prime candidate for templating the formation of isoindoline based chelates.

The second and third chapters in this thesis present the template synthesis of semihemiporphyrazines, "half" hemiporphyrazine like chelates, and alpha-amidino azadi(benzopyrro)methenes using the Re(CO)3-unit as a templating agent in a one-step reaction. In both cases, the complexes have terminal amine groups and do not experience hydrolysis as seen with the Re(CO)3-templated azadi(benzopyrro)methenes. Additionally, in the alpha-amidino azadi(benzopyrro)methene case, a rhenium bound nitrile is activated by a diiminoisoindoline unit to afford a rhenium bound amidine and one diiminoisoindoline sp 2 carbon is converted to a sp3 carbon by attack of another diiminoisoindoline unit disrupting conjugation. The spectroscopy of the semihemiporphyrazines was investigated along with DFT and TDDFT calculations. Whereas, the conjugation in the alpha-amidino azadi(benzopyrro)methenes is disrupted resulting in yellow crystalline products that lack a metal-to-ligand charge transfer band. In the third chapter, 2,6-diacetylpyridine dihydrazone is coordinated to middle and late first row transition metals and their magnetic susceptibilities are explored via Evans NMR method. In the fourth chapter, neutral and deprotonated anionic complexes of the tetrakis(perfluorophenyl)-N-confused porphyrin are prepared and investigated by UV-visible and magnetic circular dichroism spectroscopies as well as by DFT and TTDFT calculation methods.