(544ca) Single Rhodium and Palladium Atoms Anchored in Micropores for Transformation of Methane to Acetic Acid and Methanol Under Mild Condition
Catalytic transformation of CH4 under a mild condition is significant for efficient utilization of shale gas under the circumstance of switching raw materials of chemical industries to shale gas. Here we report the transformation of CH4 to acetic acid and methanol through coupling of CH4, CO and O2 on single site Rh1Om anchored in microporous aluminosilicates in solution at 150C or lower. The activity of these singly dispersed precious metal sites for production of organic oxygenates can reach about 0.10 acetic acid molecules on a Rh1On site per second at 150C with a selectivity of 70% for production of acetic acid. It is higher than the activity of free Rh cations by >1000 times. Computational studies suggest that the first C-H of CH4 is activated by Rh1O5 anchored on wall of the micropores; the formed CH3 couples with COOH species to form the first acetic acid, generating a terminal oxo structure (Rh=O). The Rh=O activates C-H of the second CH4 molecule, forming CH3 which then couples with adsorbed CO to form acetyl intermediate. The acetyl couples with adsorbed HO group, forming the second acetic acid molecule. I will also discuss the oxidation of methane to methanol on Pd1O4 sites in aqueous solution under a mild condition.
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