Abstract
Selected examples of multicopper complexes and coordination polymers applied as homogeneous catalysts or catalyst precursors in the oxidative functionalization of alkanes are described. The main types of polynuclear copper compounds are indicated, and the critical analysis of the most efficient catalytic systems is presented. The catalytic transformations concern (1) the mild oxidation of cyclohexane (model substrate) and other alkanes by H2O2 into alkyl hydroperoxides, alcohols, and ketones, and (2) the hydrocarboxylation of gaseous and liquid Cn (n = 2–9) alkanes, by CO, H2O, and K2S2O8, into the corresponding Cn + 1 carboxylic acids. The effects of important reaction parameters are highlighted and the preferable requirements for a prospective homogeneous Cu-based catalyst in oxidative transformations of alkanes are identified. These include the presence of N,O-ligands or environment, low coordination numbers of Cu centers and availability of labile ligands, high stability of the multicopper cores with relatively close separations of Cu atoms, solubility and stability of catalysts in water and/or aqueous acetonitrile medium, and their easy preparation from simple, cheap, and commercially available chemicals. Emphasis is also given to the development of alkane functionalization protocols and catalytic systems that exhibit high efficiency and selectivity, good substrate versatility, and operate under mild conditions in aqueous medium.
Published Version
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