Oxidative carbonylation of methane to acetic acid on an Fe-modified ZSM-5 zeolite

Direct catalytic conversion of methane under mild conditions is beneficial but challenging. Herein, we report a direct co-conversion of methane, carbon monoxide, and hydrogen peroxide into acetic acid, catalyzed by Fe/ZSM-5 (0.25) zeolite under mild conditions. The highest reported acetic acid space-time yield of similar to 12.01 mmol g(cat)(-1) h(-1) with an optimal selectivity of 63.2% is achieved at 50 degrees C. This relatively high yield is ascribed to the mononuclear Fe3+ species. C-13-Tracking experiments revealed that the methyl and carbonyl groups of acetic acid originate from methane and carbon monoxide, respectively. Spin-trapping experiments indicated that center dot OH and center dot CH3 radicals are involved in the reaction. In situ Raman analysis suggested that -Fe-OCH3 species is the possible intermediate. Overall, our method is greener, and our catalyst is more economical than those currently used in the industrial process. Therefore, we expect a pilot-scale test to determine the possibility as an industrial alternative.