Methane poses a threat to the environment due to its potency as a greenhouse gas [1]. Transformation of methane to methanol is one way to mitigate the problem but current methods are expensive, require high temperature and conditions as well as specialized facilities. Transition metal dication complexes have been shown to be good activators of the C-H bond of saturated hydrocarbons, an important step in methane to methanol transformation [2]. The electronic structure of transition metal oxide dications has been studied in depth to understand their behavior as either oxo or oxyl complexes [3]. With an understanding of their behavior, strong or weak field ligands (i.e. NH3 or Cl) can be added to stabilize the oxo or oxyl form respectively. In this study there are three potential reaction candidates for methane to methanol transformation, the 2+2 oxidative addition, proton coupled electron transfer (PCET), and hydrogen atom transfer (HAT). The 2+2 and PCET mechanisms utilize an oxo metal oxide and are selective for the CH bond of methane, but not efficient due to high activation energies. The HAT mechanism utilizes an oxyl metal oxide and is not selective for the CH bond, but is efficient with low energy barriers. Using multireference methods with high level basis sets, we study the effects of a varying number and combination of strong and weak field ligands on TMO2+ species to develop a suitable catalyst that will have a suitable balance for the selectivity of the CH bond and efficiency of low energy barriers.

Catalyst development for methane to methanol transformation via C-H bond activation

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