Demand for liquid transportation fuel, specifically diesel and jet fuel, as well as liquids for chemicals, is expected to grow over the next several decades and remain high long after that. Meanwhile, the global and particularly American hydrocarbon supply is steadily shifting from conventional petroleum toward shale gas and shale oil ("light tight oil"). In the longer term, demand for liquids is likely to be increasingly met with renewable and/or nuclear energy, with CO2 as the carbon source. These trends, and other potential applications, converge to create a pressing need to develop more efficient ways to make carbon-carbon (C-C) bonds to enable the conversion of small molecules to the larger hydrocarbons required for fuel and chemicals. This research will address this challenge through the development of molecular metal-based catalysts that are effective at breaking the carbon-hydrogen (C-H) bonds of saturated hydrocarbons (alkanes), and forming C-C bonds with the species thus activated. Systems developed will be based on a single catalyst that does both C-H bond cleavage and C-C bond making, or tandem systems based on two catalysts each of which effects one of the two reactions.