Computer-aided molecular design of alkane-activation catalysts. [Manganese tetra(pentafluorophenyl) porphyrin; manganese tetra(2'-carboranylphenyl-anilide) porphyrin chloride; manganese chloride derivative of tetra(2',6'-dinitrophenyl) porphyrin free base]
Our work focuses on a novel biomimetic approach to the development of catalysts for activation of methane, using computer-aided molecular design (CAMD) techniques. The biomimetic CAMD methodology consists of several elements: (1) Design activities are guided by the structural and chemical information about naturally occurring biological catalysts that carry out alkane oxidation to alcohols. The macromolecular biological catalysts are investigated to determine the features that need to be designed into a synthetic catalyst in order to mimic the alkane-oxidation function. (2) Molecular mechanics calculations are used to evaluate possible designs for catalysts based on synthetic metalloporphyrins. The metalloporphyrins have been chosen because they occur at the active site of many monooxygenases and other enzymes that catalyze C/sub 1/ chemistry. Also, the porphyrin macrocycle provides a platform upon which additional molecular architecture is erected to provide the structural features required to mimic the enzymes. (3) The computer designed catalysts are then synthesized. (4) The synthetic catalysts are characterized by various spectroscopic techniques including Raman-difference, transient Raman, FTIR, NMR, and uv-visible absorption spectroscopies. (5) The designed catalysts are tested in alkane-oxidation reactions. The activity test results and results of the structural studies are evaluated to obtain structure-activity relationships that form a basis for making further improvements in the catalyst. This feedback procedure gives an iterative method for optimizing catalytic properties. 20 refs., 3 figs.
- Research Organization:
- Sandia National Labs., Albuquerque, NM (USA)
- DOE Contract Number:
- AC04-76DP00789
- OSTI ID:
- 6917091
- Report Number(s):
- SAND-88-1045C; CONF-880912-9; ON: DE88011543
- Resource Relation:
- Conference: 196. American Chemical Society national meeting, Los Angeles, CA, USA, 25 Sep 1988; Other Information: Portions of this document are illegible in microfiche products
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
10 SYNTHETIC FUELS
ALCOHOLS
SYNTHESIS
CATALYSTS
COMPUTER-AIDED DESIGN
CYCLOHEXANE
OXIDATION
ENZYMES
CATALYTIC EFFECTS
HEXANE
MANGANESE COMPLEXES
METHANE
PORPHYRINS
CONVERSION
MOLECULAR STRUCTURE
ALKANES
CARBOXYLIC ACIDS
CHEMICAL REACTIONS
COMPLEXES
CYCLOALKANES
HETEROCYCLIC ACIDS
HETEROCYCLIC COMPOUNDS
HYDROCARBONS
HYDROXY COMPOUNDS
ORGANIC ACIDS
ORGANIC COMPOUNDS
ORGANIC NITROGEN COMPOUNDS
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