Catalytic conversion of Methane to Methanol
A critical problem in chemistry is low-temperature activation and functionalization of CH4 for both energy generation and for synthesis of useful products. Despite enormous efforts in both fundamental and applied research, available technology does not provide practical solutions to this problem. We believe that solving this problem requires a full mechanistic understanding of various processes for low temperature oxidation of CH4. Such mechanistic understanding can come only from a concerted effort using the best methods available from theory and experiment on the most promising various processes and systems.
Our approach is to elucidate the reaction mechanism of high yield alkane functionalization catalysts using experimental and theoretical chemistry methods and in parallel to utilize this information to rationally design, synthesize and characterize new catalysts. Key aspects of the proposed research will be to provide a molecular basis for both the efficiency of the catalysts being studied and their limitations. In parallel to the mechanistic studies, several new catalyst designs are proposed that we expect to be more efficient alkane heteroatom functionalization catalysts. Information from the synthesis and study of these new catalysts will strengthen our fundamental understanding of hydrocarbon heteroatom functionalization and provide a basis for an iterative process leading to the rational design of improved catalysts in this well and other fields.
Personnel: Dr. Robert (Smith) Nielsen, Dr. Marten Ahlquist, Dr. Ekaterina Tkatchouk, Mu-Jeng Cheng, Wei-Guang Liu and Patrick Theofanis.
This project is in collaboration with Dr. Roy Periana (USC) and is being supported by the ChevronTexaco Energy Research Company
- Tenn, W. J. III ; Young, K. J. H.; Bhalla, G.; Oxgaard, J.; Periana, R. A.; Goddard, W. A. III "Investigation of the Activation of C-H Bonds by an O-donor Ligated Iridium(III) Methoxo Complex" J. Am. Chem. Soc. 2005, 127, 14172 - 14173
- Bhalla, G.; Liu, X. Y.; Oxgaard, J.; Goddard, W. A. III; Periana, R. A. "Synthesis, Structure and Reactivity of O-Donor Ir(III) Complexes: C-H Activation Studies with Benzene" J. Am. Chem. Soc. 2005, 127, 11372 - 11389.
- Jones, C.; Ziatdinov, V.; Taube, D.; Periana, R. A.; Nielsen, R. J.; Oxgaard, J, Goddard, W.A. III "Selective Oxidation of Methane to Methanol Catalyzed by Homogeneous, Cationic Gold" Angew. Chem. Intl. Ed., Eng. 2004, 43, 4626 - 4629.