Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 29581429.
- Also identified by DOI 10.1038/s41467-018-03235-7 and PMC identifier 5964318.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Catalytic transformation of CH<sub>4</sub> 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<sub>4</sub> to acetic acid and methanol through coupling of CH<sub>4</sub>, CO and O<sub>2</sub> on single-site Rh<sub>1</sub>O<sub>5</sub> 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<sub>1</sub>O<sub>5</sub> 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<sub>4</sub> is activated by Rh<sub>1</sub>O<sub>5</sub> anchored on the wall of micropores of ZSM-5; the formed CH<sub>3</sub> then couples with CO and OH, to produce acetic acid over a low activation barrier.