This thesis describes the use of advanced multinuclear (13C, 1H, 29Si) solid state NMR to study the structure of heterogeneous catalyst materials with the goal of improving synthesis strategies, and gaining a better understanding of mechanisms of deactivation. This research (excluding Appendix 1) was funded through the NSF Engineering Research Center for Biorenewable Chemicals (CBiRC). It is the result of collaborative work involving several universities within the Center, including the University of New Mexico (UNM), University of Wisconsin, Madison (UW-Madison), and the Chemical Engineering Department at Iowa State University. Numerous manuscripts have resulted from these collaborations. First-author manuscripts have been added as chapters, while manuscripts with co-authorship are included as Appendices.