Carbon Monoxide Cleavage by (Silox)3Ta (Silox = (t)Bu3SiO(-)): Physical, Theoretical, and Mechanistic Investigations.

摘要

The Fischer-Tropsch (F-T) reaction, the conversion of synthesis gas (CO/H2) to hydrocarbons and oxygenates, has commanded the attention of the organometallic community for the past 10-15 years. During periods when olefin feedstocks are costly, the production of low molecular weight commodity chemical from coal or natural gas via this method becomes economically attractive. The heterogeneously catalyzed F-T process is inherently nonselective since it produces a Shulz-Flory distribution of hydrocarbons, oxygenates, or both; thus homogeneous systems, considered to possess the advantage of greater selectivity have attracted substantial interest. While a commercially feasible homogeneous F-T process has yet to be developed, some of the desired selectivity, especially toward methanol and C2 oxygenates, has been demonstrated. In addition, organometallic chemistry, through investigations of stoichiometric transformations involving carbon monoxide and dihydrogen, has dramatically increased our fundamental understanding fo plausible individual steps that pertain to the F-T reaction. (JES)