Prat, Jacob2022-09-262022-09-262022-07https://hdl.handle.net/11299/241717University of Minnesota Ph.D. dissertation. July 2022. Major: Chemistry. Advisors: Connie Lu, Ian Tonks. 1 computer file (PDF); xxviii, 222 pagesThe production of catalysts capable of the efficient and selective reactivity of CO2, H2, and CO toward useful products is required to lower global energy costs and allow for a sustainable carbon neutral future. To this end the design and synthesis of metal complexes capable of controlling the reactivity of these small molecules is highly desired. Bimetallic complexes allow for a greater chemical space allowing for high tailorability of metal catalyst properties presenting a new strategy for solving these issues. The tuning of a Z-type nickel-support bond toward small molecule reactivity unifies the chemistry described herein. In the introductory chapter the environmental and energy considerations motivating this work is made explicit. Inspired by enzymatic catalysis, a nickel-iron bimetallic complex for CO2 reduction to CO was studied in depth by NMR, Mössbauer, and electrochemical studies is detailed in Chapter 2. In Chapter 3 the role of a group 13 support on H2 binding and hydride transfer reactivity was investigated with the synthesis and characterization of a set of nickel-boron complexes. In Chapter 3 the combination of open ligand choice and metal support for the modulation of CO and CO2 binding was explored with iron and tin bimetallic nickel complexes.enBimetallicCarbon DioxideCarbon MonoxideCatalysisDihydrogenNickelThesis or Dissertation