Pyridine N-Oxide-Promoted Cobalt-Catalyzed Dioxygen-Mediated Methane Oxidation

Abstract

The partial oxidation of methane with O2 is significant due to its potential of providing abundant chemical feedstock. Only a few examples realized this type of reaction in homogeneous solvent systems, most of which are in low efficiency. Herein, we present a pyridine N-oxide-promoted cobalt-catalyzed O2-mediated methane oxidation to produce methylene bis(trifluoroacetate) with productivity over 500 molester molmetal –1 h–1.

High conversion of methane to methyl ester at 298 K

“…[25][26][27]30 Although some reaction systems show a high catalytic efficiency, over-oxidation has not been avoided. 31,32 Normally, to establish effective oxidation of methane with dioxygen to give methanol or methyl ester with a high yield under ambient conditions, it is necessary to determine: 1) a more effective catalytic species to cleave an inert C-H bond of methane (BDE = 439 kJ mol −1 ), 1 2) a reasonable way to generate methyl-oxygen intermediates using dioxygen or dioxygen activation, and 3) a chemical environment to guarantee that the product survives completely. However, because almost all the traditional powerful species, including metal complexes, non-metal compounds and enzymes, used to cleave the C-H bonds of methane are carried out in the liquid-phase or on the gas-solid interface, good solubility of solvent to methane, high partial pressure of methane, poor coordination of product molecule with reactive species and special operations in the current oxidations of methane are often required.…”

“…25–27,30 Although some reaction systems show a high catalytic efficiency, over-oxidation has not been avoided. 31,32…”