Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions

Catalytic transformation of CH(4) 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 CH(4) to acetic acid and methanol through coupling of CH(4), CO and O(2) on single-site Rh(1)O(5) anchored in microporous aluminosilicates in solution at ≤150 °C. The activity of these singly dispersed precious metal sites for production of organic oxygenates can reach about 0.10 acetic acid molecules on a Rh(1)O(5) site per second at 150 °C 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 bond of CH(4) is activated by Rh(1)O(5) anchored on the wall of micropores of ZSM-5; the formed CH(3) then couples with CO and OH, to produce acetic acid over a low activation barrier.