Use of molecular modeling to design alkane activation catalysts
Efficient alkane-activation catalysts are needed for a number of applications including methane conversion to liquid fuels, clean-up of dilute waste streams, and for oxidation of higher molecular weight alkanes, olefins, and aromatics. For some of these applications, high selectivity and regioselectively of the catalyst is desired. Our work takes a biomimetic approach to the development of shape and size selective catalysts using computer-aided molecular design (CAMD) techniques. The biomimetic CAMD methodology consists of several elements, including: (1) investigation of biological catalysts, especially those like methane monooxygenase and cytochrome P/sub 450/ that activate C-H bonds, to determine the structural features to be designed into a synthetic catalyst, (2) molecular mechanics calculations to evaluate potential catalysts, (3) synthesis of the designed catalyst, (4) spectroscopic characterization of the synthetic catalysts, and (5) catalyst testing for activity and selectivity. The activity tests and structural information provide a basis for making further improvements in the catalyst design. This biomimetic CAMD methodology is being used to design shape and size selective catalysts based on the metalloporphyrins. Designed metalloporphyrins with bulky substituents attached so as to give a small methane-binding cavity at the active metal center have been synthesized and tested. The photochemical production of the co-reductant required in the reaction that mimics cytochrome P/sub 450/ and the synthesis of bis-deep-pocket porphyrins are also described. 51 refs., 8 figs.
- Research Organization:
- Sandia National Labs., Albuquerque, NM (USA)
- DOE Contract Number:
- AC04-76DP00789
- OSTI ID:
- 6001349
- Report Number(s):
- SAND-89-1398C; CONF-890814-2; ON: DE89016185
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
10 SYNTHETIC FUELS
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
400201 -- Chemical & Physicochemical Properties
ALKANES
BIOMIMETIC PROCESSES
CARBOXYLIC ACIDS
CATALYTIC EFFECTS
CHEMICAL REACTIONS
COMPLEXES
CRYSTAL STRUCTURE
CYTOCHROMES
HETEROCYCLIC ACIDS
HETEROCYCLIC COMPOUNDS
HYDROCARBONS
METHANE
MOLECULAR STRUCTURE
ORGANIC ACIDS
ORGANIC COMPOUNDS
ORGANIC NITROGEN COMPOUNDS
OXIDATION
PHOTOCHEMICAL REACTIONS
PHOTOSENSITIVITY
PIGMENTS
PORPHYRINS
PROTEINS
SENSITIVITY
SYNTHESIS