Discrete Molecular Catalysts for Methane Functionalization

Abstract

AbstractThe implementation of selective, energy efficient, direct alkane oxidation chemistry could lead to a new paradigm in materials and energy technologies for the 21st century that is environmentally and economically superior to current processes. Such processes would allow the vast reserves of natural gas to be directly employed as feedstocks for fuels and chemicals. Molecular catalysts that activate and functionalize the CH bonds of unactivated hydrocarbons are of particular interest, from both a scientific and economic viewpoint. This results from the unique properties of these engineered materials, which allow them to carry out oxidative hydrocarbon functionalization, with high atom and energy efficiency, under relatively mild conditions. Despite the large body of work on the activation of CH bonds over the last three decades, relatively few catalyst systems based on this approach present a viable route to functionalize hydrocarbons. This dilemma is largely due to the large gaps in our fundamental knowledge to allow rational design of such catalysts. Addressed in this paper are some of the key challenges and approaches to the de novo design of alkane functionalization molecular catalysts based on the CH activation reaction, with an emphasis on our own research.