The move away from a petroleum based economy requires new materials to facilitate the move to alternative fuel sources. Safe methods of storing hydrogen gas are needed, as well as the ability to sequester carbon dioxide and other waste gases. Production of biofuels from plant materials requires efficient catalysts. Metal-organic frameworks (MOFs) are a promising class of compounds for these applications because they offer a combination of high porosity, structural integrity, and functional flexibility. The usefulness of MOFs for hydrogen gas storage and catalysis can be improved by adding active metal sites. There are two ways this can be accomplished. Firstly, one can select an organic linker with orthogonal binding affinities, meaning the affinities of the structural and functional sites are significantly different to allow the synthesis of compounds with one structural metal that defines the framework and a different metal that provides the functionality. Secondly, one can post-synthetically modify a previously synthesized MOF to add functionality that could not be incorporated into the structure during the initial synthesis. Herein, this thesis describes research into the synthesis of several MOF compounds. First, three structurally distinct cadmium linked, zinc functionalized tetrakis(carboxyphenyl)porphine compounds are synthesized and characterized. Second, metallation of an amine-containing MOF (IRMOF-3) by organolithium deprotonation followed by metal replacement is discussed.